Composition and methods for generating and sustaining molecular hydrogen (h2) in aqueous systems

ABSTRACT

Provided are compositions, methods, and solutions for generating aqueous glucomannan solutions with hydrogen compositions greater than 100 parts per billion. Said glucomannan solutions have application in nutritional, therapeutic, and energy fields.

CROSS-REFERENCE

This application is a continuation of U.S. patent application Ser. No.16/736,749 filed Jan. 7, 2020, which is a continuation of InternationalPatent Application No. PCT/US2019/042833 filed on Jul. 22, 2019, whichclaims the benefit of U.S. Provisional Application No. 62/764,222, filedJul. 23, 2018, each of which is incorporated herein by reference.

BACKGROUND

The health benefits of administering molecular hydrogen to humans andanimals by various routes, including IV, oral, transdermal, andinhalation have been. Initially, molecular hydrogen was believed tofunction as an antioxidant by direct reaction with hydroxyl radicals andperoxynitrite, while leaving the signaling reactive oxygenspecies-superoxide and hydrogen peroxide, unchanged.

Molecular hydrogen is used for wellness, anti-aging, as well asprevention and treatment of numerous diseases. Molecular hydrogen isreadily absorbed into tissues. The duration of H₂ in the body isshort-lived, since it readily diffuses in and out of tissues. Sustainingmolecular hydrogen in the tissues of humans and animals is needed forincreasing the efficacy of molecular hydrogen for reduction of tissuedamage, effects on slowing aging and slowing the progression of chronicdegenerative diseases as well as for body weight control. A means ofgenerating and retaining molecular hydrogen in the body, in a safe,economic, and consumer-friendly manner, is needed to advance its use asa therapeutic agent.

SUMMARY

Provided herein are methods of generating an aqueous glucomannansolution containing molecular hydrogen, the method comprising: providinga volume of an aqueous solvent; and adding from about 0.00001% w/v toabout 7.5% w/v glucomannan and about 0.005% to about 2.0% w/v magnesiummetal powder to the aqueous solvent, wherein the generated glucomannansolution has an increased volume which is at least 0.01%, at least 0.1%,at least 1%, at least 10%, or at least 20% greater than the volume of acorresponding glucomannan solution which does not comprise H₂; whereinthe generated glucomannan solution comprises an initial H₂ concentrationof greater than about 100 ppb (parts per billion); and wherein, uponexposure of the glucomannan solution to standard temperature andpressure (STP) for 240 minutes after its generation, the glucomannansolution comprises an H₂ concentration at least about 50% or at leastabout 70% of the initial H₂ concentration.

Provided herein are methods of generating a glucomannan solution, themethod comprising: providing a volume of an aqueous solvent; generatingor sequestering H₂ in the aqueous solvent; and adding glucomannan to theaqueous solvent, wherein the glucomannan solution has an increasedvolume which is about 0.01%, at least 0.1%, at least 1%, at least 10%,or at least 20% greater than the volume of a corresponding glucomannansolution which does not comprise H₂; wherein the generated glucomannansolution comprises an initial H₂ concentration of greater than about 100ppb (parts per billion); and wherein, upon exposure of the glucomannansolution to standard temperature and pressure (STP) for 240 minutesafter its generation, the glucomannan solution retains at least 50% ofits original concentration of H₂. Further provided are methods, whereinthe aqueous solvent comprises water. Further provided are methods,wherein the aqueous solvent is water. Further provided are methods,wherein the generated glucomannan solution has a glucomannanconcentration from about 0.00001% w/v to about 7.5% w/v. Furtherprovided are methods, wherein the generated glucomannan solution is agel. Further provided are methods, wherein the generated glucomannansolution is a flowable liquid. Further provided are methods, wherein thegenerated glucomannan solution comprises gaseous H₂. Further providedare methods, wherein, upon exposure of the glucomannan solution tostandard temperature and pressure (STP) for 240 minutes after itsgeneration, the glucomannan solution comprises an H₂ concentration atleast about 75%, at least about 80%, at least about 85%, at least about90%, at least about 95%, or at least about 99% of the initial H₂concentration. Further provided are methods, wherein the volume of thegenerated glucomannan solution comprising H₂ is at least 1% , at least10%, at least 20%, at least 30%, or at least 50% greater than the volumeof the aqueous solvent. In some methods provided herein further comprisea step of treating the aqueous solvent with electrolysis, therebygenerating H₂ in the aqueous solvent, prior to, during, or subsequent toadding the glucomannan to the aqueous solvent. Further provided aremethods, wherein the glucomannan solution comprises a base metal.Further provided are methods, wherein the aqueous solvent comprises thebase metal. Further provided are methods, wherein a base metal is addedto the aqueous solvent prior to the addition of the glucomannan to theaqueous solvent. Further provided are methods, wherein the base metal isselected from the list consisting of lithium, potassium, strontium,calcium, sodium, magnesium metal powder, aluminum, zinc, chromium,manganese, iron, and any combination thereof. Further provided aremethods, wherein the base metal is magnesium metal powder. Furtherprovided are methods, wherein the magnesium metal powder is present inthe generated glucomannan solution in an amount from about 0.00001% w/vto about 2% w/v. Further provided are methods, wherein the generatedglucomannan solution further comprises an organic acid. Further providedare methods, wherein the organic acid is selected from the listconsisting of citric acid, malic acid, lactic acid, acetic acid,tartaric acid, succinic acid, phosphoric acid or any combinationthereof. Further provided are methods, wherein the citric acid ispresent in an amount from about 0.1% w/v to about 15% w/v. Furtherprovided are methods, wherein the malic acid is present in an amountfrom about 1% (w/v) to about 50% w/v. Further provided are methods,wherein the lactic acid is present in an amount from about 1% w/v toabout 10% w/v. Further provided are methods, wherein the acetic acid ispresent in an amount from about 0.5% v/v to about 3% v/v. Furtherprovided are methods, wherein the tartaric acid is present in an amountfrom about 1% w/v to about 10% w/v. Further provided are methods,wherein the succinic acid is present in an amount from about 1% w/v toabout 10% w/v. Further provided are methods, wherein the phosphoric acidis present in an amount from about 1% v/v to about 10% v/v. Some methodsprovided herein further comprise a step of diffusing H₂ in to theaqueous solvent or the glucomannan solution from a pressurizedenvironment. Some methods provided herein further comprise a step ofexposing the generated glucomannan solution to electrolysis, therebygenerating thin the glucomannan solution. Further provided are methods,wherein the initial H₂ concentration is achieved during generation ofthe glucomannan solution. Further provided are methods, wherein theinitial H₂ concentration is achieved prior to generation of theglucomannan solution. Further provided are methods, further comprisingan isolating step, wherein bubbles in the glucomannan solution smallerthan 37 microns are isolated. Further provided are methods, wherein theisolating is by filtration. Further provided are methods, wherein theisolating is by centrifugation. Further provided are methods, whereinthe isolating is by size exclusion chromatography.

Provided herein are compositions comprising a glucomannan solution andfurther comprising hydrogen (H₂) at a concentration of greater thanabout 100 ppb (parts per billion); and wherein, upon exposure of theglucomannan solution to standard temperature and pressure (STP) for 240minutes, the concentration of hydrogen in the glucomannan solutiondeclines by less than 50% or less than 30%. Further provided herein arecompositions, further comprising an aqueous solvent. Further providedherein are compositions, wherein the aqueous solvent is water. Furtherprovided herein are compositions, wherein the concentration ofglucomannan in the glucomannan solution is from about 0.00001% w/v toabout 7.5% w/v. Further provided herein are compositions, wherein theglucomannan solution is a gel. Further provided herein are compositions,wherein the glucomannan solution is a flowable liquid. Further providedherein are compositions, wherein the H₂ is present in the glucomannansolution in a gaseous form. Further provided herein are compositions,wherein the H₂ concentration 240 minutes after generation of theglucomannan solution is at least about 75%, at least about 80%, at leastabout 85%, at least about 90%, at least about 95%, or at least about 99%of the initial H₂ concentration. Further provided herein arecompositions, wherein the volume of the glucomannan solution comprisingH₂ is at least 1% , at least 10%, at least 20%, at least 30%, or atleast 50% greater than the volume of the aqueous solvent. Furtherprovided herein are compositions, wherein the glucomannan solutioncomprises a base metal. Further provided herein are compositions,wherein the composition comprises a base metal. Further provided hereinare compositions, wherein the aqueous solvent comprises a base metal.Further provided herein are compositions, wherein the base metal isselected from the group consisting of lithium, potassium, strontium,calcium, sodium, magnesium metal powder, aluminum, zinc, chromium,manganese, iron, and any combination thereof. Further provided hereinare compositions, wherein the base metal is magnesium metal powder.Further provided herein are compositions, wherein the magnesium metalpowder is present in the glucomannan solution in an amount from about0.00001% w/v to about 2% w/v. Further provided herein are compositions,wherein the glucomannan solution further comprises an organic acid.Further provided herein are compositions, wherein the organic acid isselected from the group consisting of citric acid, malic acid, lacticacid, acetic acid, tartaric acid, succinic acid, phosphoric acid, andany combination thereof. Further provided herein are compositions,wherein the citric acid is present in an amount from about 0.1% w/v toabout 15% w/v. Further provided herein are compositions, wherein themalic acid is present in an amount from about 1% w/v to about 50% w/v.Further provided herein are compositions, wherein the lactic acid ispresent in an amount from about 1% w/v to about 10% w/v. Furtherprovided herein are compositions, wherein the acetic acid is present inan amount from about 0.5% v/v to about 3% v/v. Further provided hereinare compositions, wherein the tartaric acid is present in an amount fromabout 1% w/v to about 10% w/v. Further provided herein are compositions,wherein the succinic acid is present in an amount from about 1% w/v toabout 10% w/v. Further provided herein are compositions, wherein thephosphoric acid is present in an amount from about 1% v/v to about 10%v/v. Further provided herein are compositions, wherein the compositionis in a capsule or gel.

Provided herein are glucomannan solutions comprising a concentration ofglucomannan and hydrogen (H₂). Further provided herein are solutions,wherein the hydrogen (H₂) is present at a concentration of greater thanabout 100 ppb (parts per billion) hydrogen (H₂). Further provided hereinare solutions, wherein upon exposure to standard temperature andpressure (STP) for 240 minutes, the H₂ concentration is at least about70% of the initial H₂ concentration as measured in parts per billion(ppb). Further provided herein are solutions, wherein the glucomannanconcentration is from about 0.00001% to about 7.5%. Further providedherein are solutions, wherein the solution is a gel. Further providedherein are solutions, wherein the solution is a flowable liquid. Furtherprovided herein are solutions, wherein the H₂ is present in a gaseousform. Further provided herein are solutions, wherein, upon exposure ofthe glucomannan solution to standard temperature and pressure (STP) for240 minutes, the concentration of hydrogen in the glucomannan solutiondeclines by less than 1%, less than 5%, less than 10%, less than 15%,less than 20%, less than 25%, or less than 30%. as measured in parts perbillion (ppb). Further provided herein are solutions, wherein, uponexposure of the glucomannan solution to standard temperature andpressure (STP) for 240 minutes, the concentration of hydrogen in theglucomannan solution is at least 70% of the H₂ concentration in thesolution prior to the exposure as measured in parts per billion (ppb).Further provided herein are solutions, further comprising a base metal.Further provided herein are solutions, wherein the base metal isselected from the group consisting of lithium, potassium, strontium,calcium, sodium, magnesium metal powder, aluminum, zinc, chromium,manganese, iron, and any combination thereof. Further provided hereinare solutions, wherein the base metal is magnesium metal powder. Furtherprovided herein are solutions, wherein the magnesium metal powder ispresent in the glucomannan solution in an amount from about 0.00001% w/vto about 2% w/v. Further provided herein are solutions, furthercomprising an organic acid. Further provided herein are solutions,wherein the organic acid is selected from the list consisting of citricacid, malic acid, lactic acid, acetic acid, tartaric acid, succinicacid, phosphoric acid or any combination thereof. Further providedherein are solutions, wherein the citric acid is present in an amountfrom about 0.1% w/v to about 15% w/v. Further provided herein aresolutions, wherein the malic acid is present in an amount from about 1%(w/v) to about 50% w/v. Further provided herein are solutions, whereinthe lactic acid is present in an amount from about 1% w/v to about 10%w/v. Further provided herein are solutions, wherein the acetic acid ispresent in an amount from about 0.5% v/v to about 3% v/v. Furtherprovided herein are solutions, wherein the tartaric acid is present inan amount from about 1% w/v to about 10% w/v. Further provided hereinare solutions, wherein the succinic acid is present in an amount fromabout 1% w/v to about 10% w/v. Further provided herein are solutions,wherein the phosphoric acid is present in an amount from about 1% v/v toabout 10% v/v.

Provided herein are methods, compositions, and solutions as describedherein, further formulated for oral administration. Provided herein aremethods, compositions, and solutions as described herein, furtherformulated for rectal administration. Further provided are methods,compositions, or solutions, further formulated for oral delivery.Further provided are methods, compositions, or solutions, furtherformulated for esophageal delivery. Further provided are methods,compositions, or solutions, further formulated for gastric delivery.Further provided are methods, compositions, or solutions, furtherformulated for duodenal delivery. Further provided are methods,compositions, or solutions, further formulated for delivery to the smallintestine. Further provided are methods, compositions, or solutions,further formulated for delivery to the large intestine. Further providedare methods, compositions, or solutions, further formulated for deliveryto the colon.

Provided herein are methods, compositions, and solutions as describedherein, further formulated for parenteral delivery.

Provided herein are compositions and solutions as described herein,further formulated for a topical dosage form. Further provided hereinare compositions and solutions, wherein the topical dosage form is acream, gel, foam, ointment, lotion, or liquid.

Provided herein is a bandage comprising compositions or solutions asdescribed herein.

Provided herein is a kit for treating a skin condition, comprising: acontainer comprising a composition or solution described herein;instructions for applying the composition or solution topically to theskin.

Provided herein is a kit for treating a gastrointestinal condition,comprising: a container comprising a composition or solution asdescribed herein; and instructions for oral or rectal administration ofthe composition or solution.

Provided herein is a kit for treating an inflammatory disease,comprising: a container comprising a composition or solution asdescribed herein; and instructions for administration of the compositionor solution to treat the inflammatory disease.

Provided herein is a kit for treating obesity, comprising: a containercomprising a composition or solution as described herein; andinstructions for oral administration of the composition or solution.

Provided herein are methods for treating a skin condition, comprisingadministering a composition or solution as described herein to the skinof a subject in need thereof.

Provided herein are methods for treating a gastrointestinal condition,comprising administering a composition or solution as described herein,to a subject in need thereof.

Provided herein are methods for treating an inflammatory condition,comprising administering a composition or solution as described herein,to a subject in need thereof.

Provided herein are methods for treating obesity, comprisingadministering a composition or solution described herein, to a subjectin need thereof.

Provided herein are methods of providing H₂ as a nutritional supplementto a subject in need thereof, comprising providing a composition orsolution as described herein to a subject in need thereof.

Provided herein are methods of providing H₂ to a body or container ofwater comprising aquatic or plant life, comprising contacting the waterwith a composition or the solution as described herein.

Provided herein are methods of sequestering H₂ from an aqueous solutionin need thereof, comprising contacting the aqueous solution with acomposition or solution as described herein.

Provided herein are devices comprising a composition or solution asdescribed herein, flowably connected to a water source, allowing contactbetween the composition described herein and the water source.

Provided herein are compositions comprising a base metal andglucomannan. Further provided are compositions, wherein the base metalis selected from the list consisting of lithium, potassium, strontium,calcium, sodium, magnesium metal powder, aluminum, zinc, chromium,manganese, iron, and any combination thereof. Further provided arecompositions, wherein the base metal is magnesium metal powder. Furtherprovided are compositions, further comprising an organic acid. Furtherprovided are compositions, wherein the organic acid is selected from thelist consisting of citric acid, malic acid, lactic acid, acetic acid,tartaric acid, succinic acid, phosphoric acid or any combinationthereof. Further provided are compositions, wherein the composition isin a powder form. Further provided are compositions, wherein thecomposition is substantially free of water. Further provided arecompositions, wherein the composition is in a capsule or gel.

Provided herein are glucomannan solutions produced by a method asdescribed herein. Provided herein are methods of generating aglucomannan solution, comprising generation of a glucomannan solutionthat comprises H₂. Provided herein are methods of generating aglucomannan solution, comprising adding a magnesium metal powder andglucomannan to an aqueous solvent. Provided herein are methods ofgenerating a glucomannan solution that retains molecular hydrogen longerthan a solution without glucomannan, the method comprising: providing arelatively large volume of an aqueous solvent; adding an amount ofglucomannan to the aqueous solvent; and generating and/or infusing anamount of molecular hydrogen into the aqueous solvent, wherein theglucomannan solution has a volume from zero to more than 100% greaterthan the volume of the aqueous solvent, wherein the increase in volumeof the glucomannan solution over the aqueous solvent is dependent on theamount of glucomannan and molecular hydrogen in the glucomannansolution, wherein the generated glucomannan solution comprises aninitial H₂ concentration of greater than about 100 ppb (parts perbillion), and wherein, upon exposure of the glucomannan solution tostandard temperature and pressure for at least four hours, theglucomannan solution comprises a level of molecular hydrogen greaterthan a level of molecular hydrogen in a comparable aqueous solutionwithout glucomannan. Further provided herein are methods, wherein thegenerated glucomannan solution has a glucomannan concentration fromabout 0.00001% w/v to about 7.5% w/v. Further provided herein aremethods, wherein the generated glucomannan solution is a gel. Furtherprovided herein are methods, wherein the generated glucomannan solutionis a flowable liquid. Further provided herein are methods, wherein thegenerated glucomannan solution comprises gaseous H₂. Further providedherein are methods, wherein, upon exposure of the glucomannan solutionto standard temperature and pressure (STP) for 240 minutes after itsgeneration, the glucomannan solution comprises an H₂ concentration atleast about 75%, at least about 80%, at least about 85%, at least about90%, at least about 95%, or at least about 99% of the initial H₂concentration. Further provided herein are methods, wherein the volumeof the generated glucomannan solution comprising H₂ is at least 1% , atleast 10%, at least 20%, at least 30%, or at least 50% greater than thevolume of the aqueous solvent. Further provided herein are methods,further comprising a step of treating the aqueous solvent withelectrolysis, thereby generating H₂ in the aqueous solvent, prior toadding the glucomannan to the aqueous solvent. Further provided hereinare methods, wherein the glucomannan solution comprises a base metal.Further provided herein are methods, wherein the base metal is selectedfrom the list consisting of lithium, potassium, strontium, calcium,sodium, magnesium metal powder, aluminum, zinc, chromium, manganese,iron, and any combination thereof. Further provided herein are methods,wherein the base metal is magnesium metal powder. Further providedherein are methods, wherein the magnesium metal powder is present in thegenerated glucomannan solution in an amount from about 0.00001% w/v toabout 2% w/v. Further provided herein are methods, wherein the generatedglucomannan solution further comprises an organic acid. Further providedherein are methods, wherein the organic acid is selected from the listconsisting of citric acid, malic acid, lactic acid, acetic acid,tartaric acid, succinic acid, phosphoric acid or any combinationthereof. Further provided herein are methods, wherein the citric acid ispresent in an amount from about 0.1% w/v to about 15% w/v. Furtherprovided herein are methods, wherein the malic acid is present in anamount from about 1% (w/v) to about 50% w/v. Further provided herein aremethods, wherein the lactic acid is present in an amount from about 1%w/v to about 10% w/v. Further provided herein are methods, wherein theacetic acid is present in an amount from about 0.5% v/v to about 3% v/v.Further provided herein are methods, wherein the tartaric acid ispresent in an amount from about 1% w/v to about 10% w/v. Furtherprovided herein are methods, wherein the succinic acid is present in anamount from about 1% w/v to about 10% w/v. Further provided herein aremethods, wherein the phosphoric acid is present in an amount from about1% v/v to about 10% v/v. Further provided herein are methods, furthercomprising a step of diffusing H₂ in to the aqueous solvent or theglucomannan solution from a pressurized environment. Further providedherein are methods, further comprising a step of exposing the generatedglucomannan solution to electrolysis, thereby generating H₂ in theglucomannan solution. Further provided herein are methods, wherein aninitial H₂ concentration is achieved during generation of theglucomannan solution. Further provided herein are methods, wherein theinitial H₂ concentration is achieved prior to generation of theglucomannan solution. Further provided herein are methods, furthercomprising an isolating step, wherein bubbles in the glucomannansolution smaller than 37 microns are isolated. Further provided hereinare methods, wherein the isolating is by filtration. Further providedherein are methods, wherein the isolating is by centrifugation. Furtherprovided herein are methods, wherein the isolating is by size exclusionchromatography.

Provided herein are H₂-generating compositions comprising: lactic acid;glucomannan; magnesium metal powder; glycerin; and an aqueous solvent.Provided herein are H₂-generating compositions comprising: an organicacid; glucomannan; magnesium metal powder; glycerin; and an aqueoussolvent. Further provided herein are compositions, wherein thecomposition is a cream, gel, foam, ointment, lotion, or liquid. Providedherein are, wherein the composition is adapted for application to theskin of a subject. Provided herein are, wherein the composition providesa moisturizing effect to the skin of the subject.

INCORPORATION BY REFERENCE

All publications, patents, and patent applications mentioned in thisspecification are herein incorporated by reference to the same extent asif each individual publication, patent, or patent application wasspecifically and individually indicated to be incorporated by reference.

BRIEF DESCRIPTION OF THE DRAWINGS

The novel features of the invention are set forth with particularity inthe appended claims. A better understanding of the features andadvantages of the present invention will be obtained by reference to thefollowing detailed description that sets forth illustrative embodiments,in which the principles of the invention are utilized, and theaccompanying drawings of which:

FIG. 1 indicates the time course of molecular hydrogen (H₂) depletionfrom glucomannan solutions.

FIG. 2 indicates the time course of hydrogen generation by distilledwater electrolysis in the presence and absence of glucomannan.

FIG. 3 shows microbubbles observed in a solution 4.5 hours afterpreparation.

FIG. 4 shows microbubbles observed in a solution 8.5 hours afterpreparation.

FIG. 5A shows an exemplary housing, comprising a glucomannan gel,comprising preformed pores to allow for increased surface area ofcontact with a solution.

FIG. 5B shows an exemplary housing for a glucomannan gel, with inlet andoutlet ports to allow flow of liquid through the housing and in contactwith the glucomannan gel.

FIG. 6 shows an exemplary system comprising a device as described inFIGS. 5A and 5B and a series of pre-filters to remove particles or othercompounds.

DETAILED DESCRIPTION

Provided herein are compositions and methods to generate molecularhydrogen in aqueous compositions. The compositions provided hereinmaintain levels of molecular hydrogen (H₂) within the composition forlonger periods of time and release the molecular hydrogen more slowlythan in other compositions previously known in the art.

I. GENERATION OF MOLECULAR HYDROGEN

The concentration of hydrogen (H₂) is often reported in molarity(moles/liter (M) or millimoles/L (mM)), parts per million (ppm), partsper billion (ppb) or milligrams per liter (mg/L). In diluteconcentrations, 1 ppm is about the same as 1 mg/L and they are oftenused interchangeably. The molar mass of molecular hydrogen is about 2mg/millimole, 1 mg is approximately equivalent to 0.5 moles, therefore 1ppm=1 mg/L=0.5 mM.

The solubility of gas dissolved in water is a function of pressure andtemperature according to Henry's law:

C=P/K_(H)

where C represents the concentration of the dissolved gas (mol/L), K_(H)is a constant characteristic of the particular gas (Latm/mol), and Prepresents the partial pressure of the specific gas above the solution(atm). Given hydrogen (H₂) gas constitutes 5.5×10⁻⁵% of atmosphere, andHenry's Constant at 25° C. is 1282.05 1*atm/mol, the concentration ofhydrogen in water at 1 atmosphere is 4.29×10⁻⁷ mM, 8.65×10⁻⁷, or8.65×10⁻⁴ ppb.

Generally known methods of generating molecular hydrogen for health carepurposes include: electrolysis of water, reaction of base metals andmetal hydrides with water, direct water splitting through vibratingpiezoelectric zinc oxide microfibers in aqueous solutions, andpressurizing molecular hydrogen into water in containers resistant topermeation.

In some embodiments described herein, the molecular hydrogen isgenerated using electrolysis. Several commercial electrolysis devicesare available for generating molecular hydrogen from water. Thesedevices are limited in that they require ‘purified’ water. ‘Purified’water is defined here as water that is free of contaminants. Of mostconcern is the presence of those electrolytes in water that can formdeposits on the electrodes of the electrolysis device and render ituseless. ‘Purified’ water can be produced by distillation, reverseosmosis, ion exchange or any method that results in water that is freeof, or very low in, ions and organic contaminants. For electrolysis, thepH should be near neutral and free of electrolytes that can degrade theelectrodes. Use of electrolytes greatly reduces the lifetime ofelectrodes. A major disadvantage in using ‘purified’ water, e.g.,distilled water, is the very low output of H₂. To increase molecularhydrogen generation from ‘purified’ water, high voltage, unsafe forconsumers, is generally used.

In some embodiments described herein, the molecular hydrogen isgenerated using electrolysis.

II. GLUCOMANNAN

Konjac glucomannan is derived from the tuber of the Amorphophalluskonjac plant, which is prevalent in Asian countries including China andJapan. Glucomannan is used in preparing several types of foods.Glucomannan flour contains a variety of insoluble substances as well aswater-soluble substances. Glucomannan is a polymer composed of themonosaccharides D-glucose and D-mannose. It forms a highly viscous solwhen constituted with water at concentrations of pure glucomannan above1.0% w/w. It is the only biopolymer currently known to form an aqueousgel at room temperature. The gel forms within a few minutes of mixingwith water. U.S. Pat. No. 5,486,364 describes processes for preparingkonjac glucomannan and is incorporated herein for such disclosure. Insome embodiments, compositions described herein comprise clarifiedglucomannan that forms a clear sol with water. In some embodiments,compositions described herein comprise rapidly hydratable konjacglucomannan that is characterized by at least a 60% viscosity gain aftera 10 minute period. In some embodiments, compositions described hereincomprise chemically modified glucomannans.

Glucomannan has been used in Asia, particularly in China, for over 2,000years in applications for detoxification, tumor suppression, bloodstasis alleviation and to treat ailments such as asthma, cough, hernia,breast pain, burns as well as hematological and skin disorders.Glucomannan has additionally been shown to affect body weight reductionin animal and human studies.

In some embodiments described herein, compositions comprise from about0.0001% w/v to about 15% w/v glucomannan. In some embodiments,compositions comprise from about 0.0001% to about 0.001% glucomannan. Insome embodiments, compositions comprise from about 0.001% to about 0.01%glucomannan. In some embodiments, compositions comprise from about 0.01%to about 0.1% glucomannan. In some embodiments, compositions comprisefrom about 0.1% to about 1.0% glucomannan. In some embodiments,compositions comprise from about 1.0% to about 15% glucomannan.

III. MAGNESIUM METAL POWDER

Several base metals, for example, lithium, potassium, strontium,calcium, sodium, magnesium metal powder, aluminum, zinc, chromium,manganese and iron, when reacting with water, generate molecularhydrogen. Conditions such as temperature, or the presence of acids,bases, and other catalysts can affect the rate of the reaction.Magnesium metal powder is preferred for human consumption due to itswide margin of safety, established health benefits as an essentialelement and ease of molecular hydrogen generation under roomtemperature, atmospheric pressure, and mild acidic or basic conditions.

In some embodiments described herein, compositions comprise lithium,potassium, strontium, calcium, sodium, magnesium metal powder, aluminum,zinc, chromium, manganese, iron, or any combination thereof. In someembodiments, compositions comprise lithium. In some embodiments,compositions comprise potassium. In some embodiments, compositionscomprise strontium. In some embodiments, compositions comprise calcium.In some embodiments, compositions comprise sodium. In some embodiments,compositions comprise magnesium metal powder. In some embodiments,compositions comprise aluminum. In some embodiments, compositionscomprise zinc. In some embodiments, compositions comprise chromium. Insome embodiments, compositions comprise iron.

In embodiments described herein, compositions comprise from about 0.001%w/v to about 2% w/v of the base metal. In some embodiments, compositionscomprise from about 0.001% w/v to about 0.01% w/v of the base metal. Insome embodiments, compositions comprise from about 0.005% w/v to about0.05% w/v of the base metal. In some embodiments, compositions comprisefrom about 0.01% w/v to about 0.1% w/v of the base metal. In someembodiments, compositions comprise from about 0.05% w/v to about 0.5%w/v of the base metal. In some embodiments, compositions comprise fromabout 0.1% w/v to about 1% w/v of the base metal. In some embodiments,compositions comprise from about 0.5% w/v to about 2% w/v of the basemetal.

In some embodiments, compositions described herein comprise magnesiummetal powder (Mg). In some embodiments, compositions comprise from about0.001% to w/v to about 2% w/v magnesium metal powder. In someembodiments, compositions comprise from about 0.001% w/v to about 0.01%w/v magnesium metal powder. In some embodiments, compositions comprisefrom about 0.005% w/v to about 0.05% w/v magnesium metal powder. In someembodiments, compositions comprise from about 0.01% w/v to about 0.1%w/v magnesium metal powder. In some embodiments, compositions comprisefrom about 0.05% w/v to about 0.5% w/v magnesium metal powder. In someembodiments, compositions comprise from about 0.1% w/v to about 1% w/vmagnesium metal powder. In some embodiments, compositions comprise fromabout 0.5% w/v to about 2% w/v magnesium metal powder.

Organic acids have been shown to be effective in accelerating thegeneration of molecular hydrogen in the reaction of magnesium metalpowder with water. (See, Uan, J-Y. et. al.(2009) J. of Hydrogen Energy34 (15), 6137-6142, which is incorporated herein for such disclosure).Organic acids can include, without limitation, lactic acid, acetic acid,formic acid, citric acid, oxalic acid, uric acid, malic acid, or anycombination thereof. In some embodiments, compositions comprise lacticacid. In some embodiments, compositions comprise acetic acid. In someembodiments, compositions comprise formic acid. In some embodiments,compositions comprise citric acid. In some embodiments, compositionscomprise oxalic acid. In some embodiments, compositions comprise uricacid. In some embodiments, compositions comprise malic acid.

IV. COMMERCIAL PRODUCTS CONTAINING MAGNESIUM METAL POWDER

Products based upon magnesium metal powder, are known in the art forgenerating molecular hydrogen when reacted with water. Such productsrequire acids or catalysts to rapidly generate molecular hydrogen fromwater. These products do not have a means of sustaining molecularhydrogen in solution or in the body.

V. RATIONALE FOR USE OF MAGNESIUM METAL POWDER

In some embodiments described herein, compositions comprise magnesiummetal powder. Magnesium metal powder is safe to use for human and animalconsumption. It is stable, readily generates molecular hydrogen, isinexpensive, and is commercially available. When reacting with water, itis converted to Generally Recognized as Safe (GRAS) magnesium hydroxideaccording the reaction

Mg+2H₂O→Mg(OH)₂+H₂.

Magnesium hydroxide is an OTC drug approved laxative as well as approvedas a GRAS food additive and supplement. Magnesium is an essentialnutrient involved in over 400 enzymatic reactions in living systems.Magnesium metal reacts with water to produce molecular hydrogen and formmagnesium hydroxide. This reaction is thermodynamically favorable, andits reaction rate is pH-dependent. Ionized magnesium in a salt form, asnon-limiting examples, citrate, chloride, sulfate, or chelatedmagnesium, cannot generate molecular hydrogen in an aqueous environment.Further, covalently bound magnesium compounds such as magnesium oxide,magnesium hydroxide, magnesium carbonate cannot generate molecularhydrogen in an aqueous environment. The rate of reaction of magnesiummetal powder with water depends on several factors, some of which arediscussed below. The surface area of magnesium metal that will beexposed to water is a factor to consider. Basic physical chemistry wouldpredict that the larger the surface area, the faster and more efficientthe reaction. This otherwise obvious conclusion is modified by twofactors: First, the larger the surface area and smaller the particlesize, the more likely that magnesium metal can undergo a spontaneous andexplosive reaction with oxygen. Thus, safety is an issue. Secondly, leftalone or by a process of reducing the risk of spontaneous reaction withoxygen (or water), a magnesium oxide coat is spontaneously formed on thesurface of magnesium metal particles through a process calledpassivation. Although this coat of magnesium oxide does not greatlyreduce the amount of magnesium metal in large particles that can reactwith water, it potentially can reduce the amount of magnesium in smallparticles that can react with water. For example, the magnesium oxidecoat on nanoparticles may constitute a significant percentage of themagnesium present-reducing the amount of magnesium metal available toreact with water. All forms of magnesium metal, including but notlimited to powders, pellets, and filings, will have some reactivity withwater and oxygen. The point to be taken is that there is a particle sizedistribution of magnesium metal powder that is optimally reactive andsafe to handle under Good Manufacturing Practice (GMP) conditions.Magnesium metal powder is generally available at up to 99.999% purity,with aluminum being the main impurity.

The size distribution of magnesium metal powder used in the studiesdescribed herein was determined using Fieldmaster® Sieves of 35, 60,120, and 230 Mesh, corresponding, respectively to 500, 250, 125 and 63microns. The size distribution was found to be: 0.7% equal to or greaterthan 500 microns; 1.2% 250-500 microns; 9.3% 125-250 microns; 38.2% at63-125 microns, and 50.9% smaller than 63 microns.

VI. MAGNESIUM METAL POWDER PLUS GLUCOMANNAN POWDER

The reaction rate of magnesium metal powder with water in the presenceof glucomannan is described herein, and depends on several factors,including pH and the presence of catalysts. For forming gels usingmagnesium metal powder-glucomannan complexes, a fast rate of molecularhydrogen production is not necessarily desirable. That is, moremolecular hydrogen will be sequestered in the gel if the gel is formedbefore a significant percentage of the available molecular hydrogen isgenerated.

As is well known in the art, variation of pH from neutrality canaccelerate the reaction of magnesium metal with water. Acidic conditionscan include any organic or inorganic acid that lowers the pH below 7.0.Included are gastric fluids, acidic foods, and acidic aquaticenvironments. Examples of acids and/or their salts that can be usedinclude citric acid, malic acid, adipic acid, fumaric acid, succinicacid, ascorbic acid, iso-ascorbic acid, salicylic acid, phosphoric acid,potassium sorbate and sodium bisulfite. Examples of antioxidants, thatare salts of acids, include sodium ascorbate and potassium ascorbate. Onthe alkaline side, magnesium oxide, magnesium hydroxide, potassium andsodium hydroxide can be used to increase the pH to alkaline conditions.Combinations of these agents can be used to control the rates ofreaction of magnesium metal in aqueous glucomannan at conditions thatgenerate H₂ in solutions and gels.

In some embodiments described herein, compositions comprise an acid orantioxidant catalyst. In some embodiments, the compositions areformulated for oral administration for gastric delivery. In someembodiments, the oral formulation comprises capsules, powder, tablets oranother delivery vehicle. In some embodiments, the compositionformulation for gastric delivery utilizes the acidity of stomach fluidto catalyze the reaction of magnesium metal or a magnesium hydride withwater to form the molecular hydrogen-rich solution or a viscous solutionor a gel. Also, when adding a magnesium metal powder-glucomannanformulation to acidic products, such as tea or acidic beverages, theacidity of the product is more than sufficient to catalyze the reactionof water with magnesium metal powder to generate molecular hydrogen. Insome embodiments, the composition comprises a base, for example, sodiumbicarbonate, to modulate the reaction.

It has been found that when combining magnesium metal powder andglucomannan and mixing with water-that a hydrogen-rich solution, viscoussolution or expansive gel with unexpected high sustainability ofmolecular hydrogen is created. Depending on the concentrations ofmagnesium metal powder and glucomannan, the pH and activity of water—theresulting solutions and gel-like structures display the following novelproperties:

1. In a closed plastic container, at ambient temperature, molecularhydrogen remains in glucomannan solutions and gels, at a level of up to60% of the original molecular hydrogen content - for over 39 days. (Ref:Table 3).

2. In a closed plastic container, at 1-4 degrees centigrade, molecularhydrogen remains in a glucomannan gel, at a level of up to 51% of theoriginal H₂ content—for over 73 days. (Ref: Table 6)

3. In an open plastic container, at room temperature, molecular hydrogenremains in 0.15 to 1,000 mg/100 mL non-gelling, low viscosity aqueoussolutions of glucomannan, at a level of up to 99% of the original H₂content—for over 15 days. (Ref: Table 14)

4. In an open plastic container, at room temperature, molecular hydrogenremains in viscous glucomannan solutions, at a level of up to 50% of theoriginal molecular hydrogen content—for over 15 days. (Ref: FIG. 1,Table 14).

5. When magnesium metal powder reacts with water in the presence of1-10% glucomannan, it generates molecular hydrogen which expands theresultant aqueous gel by up to 83% v/v—depending on the pH andconcentration of the constituents. (Ref: Table 2).

6. H₂ sequestration by magnesium metal powder-glucomannan gels createsaqueous gels of various density and porosity thereby affecting adesirable ‘fluffy’ texture-depending of the concentration of the basicconstituents. (Ref: Tables 1 and 10).

7. Great tasting, ‘fluffy’ textured, nutritious aqueous magnesium metalpowder-glucomannan gels, with health benefits, can be created byincorporating one or more of the following into the gels: sweeteners,flavoring agents, natural fruit and vegetable powders, tea powders,protein powders, vitamin powders, probiotic powders, prebiotics, drugsand nutritional supplements. (Ref: Tables 8 and 10).

8. Glucomannan, in aqueous solution, increases the yield of molecularhydrogen generation by affecting removal of the passivation coat ofmagnesium oxide from the surface of magnesium metal. (Ref: Table 14,FIG. 1).

9. Exposing aqueous solutions or gels of glucomannan to molecularhydrogen allows the sequestration of molecular hydrogen by glucomannan.(Ref: Table 15, FIG. 2).

10. Long lasting H₂ microbubble stability in non-viscous magnesium metalpowder-glucomannan solutions, in an open system, at room temperature.

11. Creation of H₂ sustained release gels, of various rates of release,for nutrients, drugs and beneficial environmental factors, including H₂.

Furthermore, it has been conceived that the resulting molecularhydrogen-glucomannan gels and viscous solutions can be utilized to:

1. Provide extended, long lasting delivery of molecular hydrogen to thebody of mammals through its persistence in the gastrointestinal tractand other tissues—such as skin;

2. Use of this biotechnology to produce hydrogen-rich magnesium metalpowder-glucomannan gels that are low calorie, good tasting, filling, andlong lasting due to floating and expanding in the upper G-Itract—properties that are useful for augmentation of fasting,anti-inflammatory, and weight control programs.

3. Provide molecular hydrogen-generating capsules or tablets, takenorally, that support weight control and fasting regimens by forming anexpanded, floating gel in the aqueous acidic environment of thestomach—while reducing the inflammatory complications of obesity.

4. Provide extended, long lasting delivery of molecular hydrogen (H₂) tothe oral cavity of humans and animals to treat plaque build-up,gingivitis, periodontal disease, and other inflammatory conditions ofthe oral cavity, esophagus and stomach.

5. H₂ generating magnesium metal powder-glucomannan gels that act as asustained drug-delivery system in the upper G-I tract—for drugs thatneed to be held in the stomach for an extended period or need to beslowly released into the systemic circulation. Molecular hydrogenrelease will act synergistically with some of these drugs. Drugs thatcan eradicate Helicobacter pylori from the upper G-I Tract, treat andprevent gastric and duodenal ulcers, treat GERD are of most interest.Gel delivery of bismuth subsalicylate, with and without other drugs totreat G-I afflictions and infections is of interest.

6. Act as an extended release system for topical delivery of molecularhydrogen to dermal tissues for treatment of infections and inflammatorydiseases.

7. Drugs delivered topically, for an extended time—or need to be slowlyreleased into the systemic circulation. Hydrogen release will actsynergistically with some of these drugs.

8. Enhanced growth and seed germination for aquatic plant, crustaceanand fish life by providing a sustained release gel system for bothmolecular hydrogen and nutrients into aquatic systems.

9. Enhanced growth rates for farming of insects by providing a sustainedrelease gel system for both molecular hydrogen and nutrients needed foraccelerated growth.

10. Act both as a generator and storage vehicle for molecular hydrogenthat can be used as a fuel, when harvested from the gel.

VII. MAGNESIUM METAL POWDER-GLUCOMANNAN GELS WITH EXCIPIENTS ANDFUNCTIONAL AGENTS

In some embodiments described herein, compositions comprise additionalexcipients or functional agents. Excipients or functional agent includedin some compositions described herein comprise sweeteners, flavoringagents, natural fruit and vegetable powders, tea powders, proteinpowders, vitamin powders, probiotic powders, anti-caking agents,preservatives, prebiotics, nutritional supplements, drugs, and foodcolorings.

In some embodiments, compositions comprise sweeteners, alone or incombination, including, but not limited to, acesulfame, aspartame,saccharin, sucralose, sucrose, monk fruit, glucose, fructose, xylitol,mannitol, glycerin, maltodextrin, inulin, and erythritol. Compositionsdescribed herein may contain sweeteners, alone or in combination, in aconcentration of from about 0.1 to about 20% w/w of the composition.Compositions described herein may contain sweeteners, alone or incombination, in a concentration of about 0.1%, about 0.2%, about 0.3%,about 0.4%, about 0.5%, about 0.6%, about 0.7%, about 0.8%, about 0.9%,about 1%, about 2%, about 3%, about 4%, about 5%, about 6%, about 7%,about 8%, about 9%, about 10%, about 12%, about 14%, about 16%, about18%, about 20%, from about 0.1% to about 5%, from about 1% to about 10%,from about 5% to about 15%, or from about 10% to about 20%, or fromabout 0.1% to about 20% w/w of the composition.

In some embodiments, compositions comprise flavoring agents, alone or incombination, including, but not limited to, natural lemon powder, citricacid, malic acid, hydroxy-citric acid, tartaric acid, adipic acid,vanillin, chocolate, cherry, pomegranate, raspberry, and strawberryflavoring. Compositions described herein may contain flavoring agents,alone or in combination, in a concentration of about 0.1%, about 0.2%,about 0.3%, about 0.4%, about 0.5%, about 0.6%, about 0.7%, about 0.8%,about 0.9%, about 1%, about 2%, about 3%, about 4%, about 5%, about 6%,about 7%, about 8%, about 9%, about 10%, about 12%, about 14%, about16%, about 18%, about 20%, %, about 25%, about 30%, about 35%, about40%, about 45%, about 50%, from about 0.1% to about 5%, from about 1% toabout 10%, from about 5% to about 15%, or from about 10% to about 20%,from about 15% to about 25%, from about 20% to about 30%, from about 25%to about 35%, from about 30% to about 40%, from about 35% to about 45%,from about 40% to about 50%, or from about 0.1% to about 50% w/w of thecomposition.

In some embodiments, compositions comprise water extracts of naturalfruit powders, alone or in combination, including, but not limited to,bilberry, lemon, blueberry, cranberry, cinnamon, ginger, lemon balm,vanilla, pumpkin seed and strawberry. Compositions described herein maycontain water extracts of natural fruit powders, alone or incombination, in a concentration of about 0.1%, about 0.2%, about 0.3%,about 0.4%, about 0.5%, about 0.6%, about 0.7%, about 0.8%, about 0.9%,about 1%, about 2%, about 3%, about 4%, about 5%, about 6%, about 7%,about 8%, about 9%, about 10%, about 12%, about 14%, about 16%, about18%, about 20%, %, about 25%, about 30%, about 35%, about 40%, about45%, about 50%, from about 0.1% to about 5%, from about 1% to about 10%,from about 5% to about 15%, or from about 10% to about 20%, from about15% to about 25%, from about 20% to about 30%, from about 25% to about35%, from about 30% to about 40%, from about 35% to about 45%, fromabout 40% to about 50%, or from about 0.1% to about 50% w/w of thecomposition.

In some embodiments, compositions comprise water extracts of naturalvegetable powders, alone or in combination, including, but not limitedto, carrot juice, spinach, broccoli, sweet potato and white willow barkpowder. Compositions described herein may contain water extracts ofnatural vegetable powders, alone or in combination, in a concentrationof about 0.1%, about 0.2%, about 0.3%, about 0.4%, about 0.5%, about0.6%, about 0.7%, about 0.8%, about 0.9%, about 1%, about 2%, about 3%,about 4%, about 5%, about 6%, about 7%, about 8%, about 9%, about 10%,about 12%, about 14%, about 16%, about 18%, about 20%, %, about 25%,about 30%, about 35%, about 40%, about 45%, about 50%, from about 0.1%to about 5%, from about 1% to about 10%, from about 5% to about 15%, orfrom about 10% to about 20%, from about 15% to about 25%, from about 20%to about 30%, from about 25% to about 35%, from about 30% to about 40%,from about 35% to about 45%, from about 40% to about 50%, or from about0.1% to about 50% w/w of the composition.

In some embodiments, compositions comprise herbal tea water extractpowders, alone or in combination, including, but not limited to, whitetea, green tea, Red Gush Chai, Matcha, Maca, Kombucha, Turmeric,Dandelion, Ginger, Lemon Ginger, Oolong, Rooibos, Fennell, Nettle Leaf,Peppermint, Echinacea, Valerian, Cinnamon Berry, Chamomile and Lavendertea. Compositions described herein may contain herbal tea water extractpowders, alone or in combination, in a concentration of about 0.1%,about 0.2%, about 0.3%, about 0.4%, about 0.5%, about 0.6%, about 0.7%,about 0.8%, about 0.9%, about 1%, about 2%, about 3%, about 4%, about5%, about 6%, about 7%, about 8%, about 9%, about 10%, about 12%, about14%, about 16%, about 18%, about 20%, %, about 25%, about 30%, about35%, about 40%, about 45%, about 50%, about 55%, about 60%, about 65%,about 70%, from about 0.1% to about 5%, from about 1% to about 10%, fromabout 5% to about 15%, or from about 10% to about 20%, from about 15% toabout 25%, from about 20% to about 30%, from about 25% to about 35%,from about 30% to about 40%, from about 35% to about 45%, from about 40%to about 50%, from about 45% to about 55%, from about 50% to about 60%,from about 55% to about 65%, from about 60% to about 70%, or from about0.1% to about 70% w/w of the composition.

In some embodiments, compositions comprise protein powders, alone or incombination, including, but are not limited to, non-fat milk, 1% fatmilk, 2% fat milk, whole milk, goat milk, rice milk, almond milk, soymilk, coconut, pea protein and brown rice protein. Compositionsdescribed herein may contain protein powders, alone or in combination,in a concentration of about 0.2%, about 0.3%, about 0.4%, about 0.5%,about 0.6%, about 0.7%, about 0.8%, about 0.9%, about 1%, about 2%,about 3%, about 4%, about 5%, about 6%, about 7%, about 8%, about 9%,about 10%, about 12%, about 14%, about 16%, about 18%, about 20%, %,about 25%, about 30%, about 35%, about 40%, about 45%, about 50%, fromabout 0.2% to about 5%, from about 1% to about 10%, from about 5% toabout 15%, or from about 10% to about 20%, from about 15% to about 25%,from about 20% to about 30%, from about 25% to about 35%, from about 30%to about 40%, from about 35% to about 45%, from about 40% to about 50%,or from about 0.2% to about 50% w/w of the composition.

In some embodiments, compositions comprise vitamins or minerals, aloneor in combination, including, but are not limited to, vitamin A, vitaminC, calcium, iron, vitamin D3, vitamin E, thiamin, riboflavin, niacin,vitamin B6, Folate, vitamin B12, biotin, pantothenic acid, phosphorous,iodine, magnesium metal powder, zinc, selenium, copper, manganese andchromium. Compositions described herein may contain vitamins orminerals, alone or in combination, in an amount of about 5%, about 6%,about 7%, about 8%, about 9%, about 10%, about 12%, about 14%, about16%, about 18%, about 20%, %, about 25%, about 30%, about 35%, about40%, about 45%, about 50%, about 55%, about 60%, about 65%, about 70%,about 75%, about 80%, about 85%, about 90%, about 95%, about 100%, fromabout 5% to about 15%, or from about 10% to about 20%, from about 15% toabout 25%, from about 20% to about 30%, from about 25% to about 35%,from about 30% to about 40%, from about 35% to about 45%, from about 40%to about 50%, from about 45% to about 55%, from about 50% to about 60%,from about 55% to about 65%, from about 60% to about 70%, from about 65%to about 75%, from about 70% to about 80%, from about 75% to about 85%,from about 80% to about 90%, from about 85% to about 95%, from about 90%to about 100%, or from about 5% to about 100% of the RDI (Required DailyIntake) for a healthy adult human.

In some embodiments, compositions comprise probiotics, alone or incombination, including, but not limited to Bacillus coagulans, Bacillussubtilis, Bacillus infantis, Lactobacillus longum, Lactobacillus casei,Lactobacillus acidophilus and Bifidobacterium. Compositions describedherein may contain probiotics, alone or in combination, in an amount ofabout 0.1%, about 0.2%, about 0.3%, about 0.4%, about 0.5%, about 0.6%,about 0.7%, about 0.8%, about 0.9%, about 1%, about 2%, about 3%, about4%, about 5%, about 6%, about 7%, about 8%, about 9%, about 10%, fromabout 0.1% to about 5%, from about 1% to about 10%, from about 5% toabout 15%, or from about 10% to about 20%, from about 15% to about 25%,from about 20% to about 30%, from about 25% to about 35%, from about 30%to about 40%, from about 35% to about 45%, from about 40% to about 50%,or from about 0.1% to about 10% w/w of the composition.

In some embodiments, compositions comprise anti-caking agents, alone orin combination, including, but not limited to, calcium phosphatetribasic, calcium silicate, sodium alginate, cellulose, microcrystallinecellulose, xanthan gum, magnesium carbonate, magnesium oxide, magnesiumsilicate, and magnesium sulfate. Compositions described herein maycontain anti-caking agents, alone or in combination, in a concentrationof about 0.1%, about 0.2%, about 0.3%, about 0.4%, about 0.5%, about0.6%, about 0.7%, about 0.8%, about 0.9%, about 1%, about 2%, about 3%,about 4%, about 5%, from about 0.1% to about 2%, from about 0.5% toabout 3%, from about 1% to about 4%, from about 2% to about 5%, or fromabout 0.1% to about 5% w/w of the composition.

In some embodiments, compositions comprise preservatives, alone or incombination, including, but not limited to, ascorbic acid, calciumascorbate, erythorbic acid, sodium ascorbate, sodium erythorbate,benzoic acid, calcium sorbate, potassium sorbate, sorbic acid, citricacid, L-cysteine, lecithin, tartaric acid and tocopherols. Compositionsdescribed herein may contain preservatives, alone or in combination, ina concentration of about 0.1%, about 0.2%, about 0.3%, about 0.4%, about0.5%, about 0.6%, about 0.7%, about 0.8%, about 0.9%, about 1%, about2%, about 3%, about 4%, about 5%, about 6%, about 7%, about 8%, about9%, about 10%, from about 0.1% to about 4%, from about 1% to about 7%,from about 3% to about 10%, or from about 0.1% to about 10% w/w of thecomposition.

In some embodiments, compositions comprise prebiotics, alone or incombination, including, but not limited to, psyllium, rice hulks,chicory root, dandelion greens, apples, bananas, artichokes, leeks, andasparagus. Compositions described herein may contain prebiotics, aloneor in combination, in a concentration of about 0.1%, about 0.2%, about0.3%, about 0.4%, about 0.5%, about 0.6%, about 0.7%, about 0.8%, about0.9%, about 1%, about 2%, about 3%, about 4%, about 5%, about 6%, about7%, about 8%, about 9%, about 10%, about 12%, about 14%, about 16%,about 18%, about 20%, %, about 25%, about 30%, about 35%, about 40%,about 45%, about 50%, about 55%, about 60%, about 65%, about 70%, about75%, from about 0.1% to about 5%, from about 1% to about 10%, from about5% to about 15%, or from about 10% to about 20%, from about 15% to about25%, from about 20% to about 30%, from about 25% to about 35%, fromabout 30% to about 40%, from about 35% to about 45%, from about 40% toabout 50%, from about 45% to about 55%, from about 50% to about 60%,from about 55% to about 65%, from about 60% to about 70%, from about 65%to about 75%, or from about 0.1% to about 75% w/w of the composition.

In some embodiments, compositions comprise nutritional supplements,alone or in combination, including, but not limited to, L-arginine,L-ornithine, 5-hydroxytryptophan, acetyl L-tyrosine, acetyl-L carnitine,alpha-lipoic acid, ashwagandha, bacopa, berbine, betaine, biotin,choline, creatine, curcumin, fish oil, flaxseed oil, ginger, ginseng,jiaogulan, kelp, manganese, methyl folate, N-acetyl-cysteine,nattokinase, niacin, quercetin, resveratrol, L-theanine, valerian root,vinpocetine and melatonin. Compositions described herein may containnutritional supplements, alone or in combination, in a concentration ofabout 0.01%, about 0.02%, about 0.03%, about 0.04%, about 0.05%, about0.06%, about 0.07%, about 0.08%, about 0.09%, about 0.1%, about 0.2%,about 0.3%, about 0.4%, about 0.5%, about 0.6%, about 0.7%, about 0.8%,about 0.9%, about 1%, about 2%, about 3%, about 4%, about 5%, about 6%,about 7%, about 8%, about 9%, about 10%, about 12%, about 14%, about16%, about 18%, about 20%, %, about 25%, about 30%, from about 0.01% toabout 0.5%, from about 0.1% to about 5%, from about 1% to about 10%,from about 5% to about 15%, or from about 10% to about 20%, from about15% to about 25%, from about 20% to about 30%, or from about 0.01% toabout 30% w/w of the composition.

In some embodiments, compositions comprise over the counter (OTC) andprescription (Rx) drugs, alone or in combination, including, but notlimited to salicylic acid, trans-retinoic acid, the alpha-hydroxy acids(e.g., lactic acid), benzoyl peroxide, bismuth subsalicylate,metronidazole, tetracycline, erythromycin, proton pump inhibitors,misoprostol, antibiotics, anti-fungal drugs, anti-inflammatories, orantacids. Compositions described herein may contain over the counter(OTC) and prescription (Rx) drugs, alone or in combination, in an amountof about 0.1%, about 0.2%, about 0.3%, about 0.4%, about 0.5%, about0.6%, about 0.7%, about 0.8%, about 0.9%, about 1%, about 2%, about 3%,about 4%, about 5%, about 6%, about 7%, about 8%, about 9%, about 10%,about 15%, about 20%, from about 0.1% to about 5%, from about 1% toabout 10%, from about 5% to about 15%, from about 10% to about 20%, orfrom about 0.1% to about 20% w/w of the composition.

In some embodiments, compositions comprise food colorings, alone or incombination, including, but not limited to FD&C Blue #1, FD&C Blue #2,FD&C Green #3, FD&C Red #3, FD&C Yellow #5, FD&C Yellow #6, riboflavin,annatto, carmine, elderberry juice powder, lycopene, or turmeric.Compositions described herein may contain food colorings, alone or incombination, in an amount of about 0.001 ppm, about 0.002 ppm, about0.003 ppm, about 0.004 ppm, about 0.005 ppm, about 0.006 ppm, about0.007 ppm, about 0.008 ppm, about 0.009 ppm, about 0.01 ppm, about 0.02ppm, about 0.03 ppm, about 0.04 ppm, about 0.05 ppm, about 0.06 ppm,about 0.07 ppm, about 0.08 ppm, about 0.09 ppm, about 0.1 ppm, about 0.2ppm, about 0.3 ppm, about 0.4 ppm, about 0.5 ppm, about 0.6 ppm, about0.7 ppm, about 0.8 ppm, about 0.9 ppm, about 1 ppm, about 2 ppm, about 3ppm, about 4 ppm, about 5 ppm, about 6 ppm, about 7 ppm, about 8 ppm,about 9 ppm, about 10 ppm, about 20 ppm, about 30 ppm, about 40 ppm,about 50 ppm, about 60 ppm, about 70 ppm, about 80 ppm, about 90 ppm,about 100 ppm, about 200 ppm, about 300 ppm, about 400 ppm, about 500ppm, from about 0.001 ppm to about 0.05 ppm, from about 0.05 ppm toabout 0.1 ppm, from about 0.1 ppm to about 0.5 ppm, from about 0.5 ppmto about 1 ppm, from about 0.5 ppm to about 5 ppm, from about 1 ppm toabout 10 ppm, from about 5 ppm to about 50 ppm, from about 50 ppm toabout 200 ppm, from about 100 ppm to about 500 ppm, or from about 0.001ppm to about 500 ppm w/w of the composition.

VIII. FORMATION AND CHARACTERISTICS OF MOLECULAR HYDROGEN GENERATING ANDSUSTAINING GLUCOMANNAN GELS

It has been unexpectedly found that when magnesium metal powder iscombined with glucomannan powder in a powder formulation and then mixedwith water, a gel is created that has some novel properties, includinggenerating, holding, and sustaining large volumes of molecular hydrogenfor an extended period of time. The resultant gels have low density andhigh porosity, as noted by observing the molecular hydrogen ‘bubble’content and measuring the dissolved molecular hydrogen. Thesecharacteristics allow for formulating gels that are nutritious and havea desirable texture as a food as well as other applications. There arehealth benefits such as use as an adjunct to weight control and fastingregimens. The effect of retaining large quantities of molecular hydrogenin glucomannan gels is non-obvious since it is shown that generation ofcarbon dioxide in a glucomannan gel does not retain that gas in the gelnor change its density (See Rows 2-5, Table 1). Also, preparing controlaqueous glucomannan gels in air (i.e., with 20% oxygen), i.e.,glucomannan without magnesium metal powder in air does not retain gasbubbles of expand the aqueous glucomannan gel.

TABLE 1 Effect of CO₂ or H₂ gas generation on glucomannan gel densityGel Head Total H₂ Final Gel/g Row Formulas in 000 Capsules/Aq. AceticAcid mL mL mL ppm pH gmn Capsules Potassium Bicarbonate Study 1 0.1 g Mg0.0 37.6 37.6 0.7 3.4 0.0 1 2 0.1 g K bicarbonate. + 2.0 g gmn 13.4 0.013.4 0.0 3.3 6.7 3 3 0.2 g K bicarbonate. + 2.0 g gmn 21.6 9.3 30.9 0.03.2 10.8 3 4 0.4 g K bicarbonate. + 2.0 g gmn 11.0 10.3 21.3 0.0 3.4 5.54 5 0.8 g K bicarbonate. + 2.0 g gmn 11.4 14.3 25.7 0.0 3.7 7.2 4 0.1 gMagnesium Metal Powder Study 6 1.6 g gmn 18.8 0.0 18.8 0.0 2.9 11.8 3 70.1 g Mg + 0.8 g K bicarbonate, 2.0 g gmn 45.5 39.4 84.9 1.3 3.9 22.8 39 0.05 g Mg + 1.6 g gmn 49.2 14.2 63.4 0.6 3.4 30.8 2 8 0.1 g Mg + 3.0 ggmn 75.1 22.7 97.8 0.8 3.4 25.0 5 10 0.15 g Mg + 4.0 g gmn 132.7 25.4158.1 2.2 3.7 33.2 7 Glucomannan Reduction of Passivation 11 0.1 g Mg +0.2 g gmn 17.6 26.9 43.0 1.0 3.4 88.0 1 12 0.1 g Mg + 0.4 g gmn 24.425.4 49.8 0.9 3.4 61.0 1 13 0.1 g Mg + 0.8 g gmn 41.6 28.8 70.4 1.2 3.352.0 2 14 0.1 g Mg + 1.6 g gmn 73.4 22.5 95.9 1.5 3.5 45.9 3 15 0.1 gMg + 1.6 g gmn (Repeat) 73.3 25.7 99.0 1.0 3.4 45.8 3 Abbreviations H₂:Molecular Hydrogen Mg: Magnesium metal powder gmn: Konjac glucomannanK—potassium Gel Vol. Volume occupied by glucomannan gel Headspace:Volume (mL) of H₂ gas displacing water in the headspace of the sealed500 mL bottle. Total Vol.: Volume occupied by the glucomannan gel andheadspace volume.

As listed in Table 2 and Table 3, formulas were prepared containing 0 to207 mg of crude magnesium metal powder (Mg), 0 to 8.0 grams of konjacroot glucomannan and 0 to 7 grams of citric acid. As listed in Table 4,powders containing magnesium metal, glucomannan (gmn), and citric acidwere prepared using a gravimetric method.

TABLE 2 Effect of Varying Components of Magnesium Metal Powder -Glucomannan Formulations Total Bubble Formulas/100 mL DW Gel Dens. H₂ mLH₂/ Gel Gel Row Vary Magnesium Metal Powder g/mL mL mg Mg (mL) Vol. 14.0 g gmn + 5.0 g CA(Reference) 0.994 xxxxx xxxx 112.8 0.0 2 11 mg Mg +4.0 g gmn + 5.0 g CA 0.825 16.6  1.51 129.4 129.4 3 24 mg Mg + 4.0 ggmn + 5.0 g CA 0.751 29.9  1.25 142.7 142.7 4 42 mg Mg + 4.0 g gmn + 5.0g CA 0.734 32.8  0.78 146.0 146.0 5 63 mg Mg + 4.0 g gmn + 5.0 g CA0.704 39.8  0.63 152.6 152.6 6 207 mg Mg + 4.0 g gmn + 5.0 g CA 0.54783.0  0.40 195.8 195.8 Total Bubble Gel Dens. H₂ mL H₂/ Gel Gel VaryCitric Acid (CA) g/mL mL g CA (mL) Vol. 7 4.0 g gmn (Ref.) 0.879 xxxxxxxxxx 112.8 0 8 0.1 g Mg + 4.0 g gmn 0.879  3.3 xxxxx 116.1 116.1 9 4.0g gmn + 0.5 g CA (Ref.) 0.969 xxxxx xxxxx 116.1 0 10 0.1 g Mg + 4.0 ggmn + 0.5 g CA 0.735 23.3 46.6  139.4 139.4 11 4.0 g gmn + 1.0 g CA(Ref.) 0.861 xxxxx xxxxx 119.5 0 12 0.1 g Mg + 4.0 g gmn + 1.0 g CA0.690 29.8 29.8  149.3 149.3 13 4.0 g gmn + 2.0 g CA (Ref.) 0.954 xxxxxxxxxx 119.5 0 14 0.1 g Mg + 4.0 g gmn + 2.0 g CA 0.682 33.1 16.6  152.6152.6 15 4.0 g gmn + 4.0 g CA (Ref.) 0.913 xxxxx xxxxx 116.1 0 16 0.1 gMg + 4.0 g gmn + 4.0 g CA 0.624 53.1 13.3  169.2 169.2 17 8.0 g gmn +7.0 g CA (Ref.) 0.986 xxxxx xxxxx 116.1 0 18 0.1 g Mg + 8.0 g gmn + 7.0g CA 0.640 59.8 8.5 175.9 175.9 Total Bubble Gel Dens. H₂ mL H₂/ Gel GelVary Glucomannan (gmn) g/mL mL g gmn (mL) Vol. 19 0.5 g gmn + 5.0 gCA/DW (Ref.) 0.916 xxx xxx 112.8 0 20 0.1 g Mg + 0.5 g gmn + 5.0 g CA/DW0.677 39.8 79.6  152.6 59.7 21 1.0 g gmn + 5.0 g CA/DW (Ref.) 0.916 xxxxxx 112.8 0 22 0.1 g Mg + 1.0 g gmn + 5.0 g CA/DW 0.710 33.2 33.2  146.0146.0 23 2.0 g gmn + 5.0 g CA/DW (Ref.) 0.854 xxx xxx 122.8 0 24 0.1 gMg + 2.0 g gmn + 5.0 g CA/DW 0.787  9.9 5.0 132.7 132.7 25 3.0 g gmn +5.0 g CA/DW (Ref.) 0.842 xxx xxx 126.0 0 26 0.1 g Mg + 3.0 g gmn + 5.0 gCA/DW 0.778 10.1 3.4 136.1 136.1 27 4.0 g gmn + 5.0 g CA/DW (Ref.) 0.895xxx xxx 119.5 0 28 0.1 g Mg + 4.0 g gmn + 5.0 g CA/DW 0.648 36.5 9.1156.0 156.0 29 6.0 g gmn + 5.0 g CA/DW (Ref.) 0.943 xxx xxx 114.5 0 300.1 g Mg + 6.0 g gmn + 5.0 g CA/DW 0.762 28.2 4.7 142.7 142.7 31 8.0 ggmn + 5.0 g CA/DW (Ref.) 0.985 xxx xxx 112.8 0 32 0.1 g Mg + 8.0 g gmn +5.0 g CA/DW 0.668 53.1 6.6 165.9 165.9 33 8.0 g gmn + 7.0 g CA/DW (Ref.)0.986 xxx xxx 114.5 0 34 0.1 g Mg + 8.0 g gmn + 7.0 g CA/DW 0.640 61.47.7 175.9 175.9 Abbreviations Mg: magnesium metal powder gmn:glucomannan CA: citric acid DW: distilled water Dens: Density; Vol.:Volume

TABLE 3 Room Temperature (23 C.) Stability of Molecular Hydrogen (H₂) inMagnesium Metal Powder - Glucomannan Gels Study Extended from Table 2BGV BGV BGV BGV BGV BGV Formulas/100 mL DW 1-Hr. 53-Hr. 108-Hr. 180-Hr.204-Hr. 261-Hr. 1 4.0 g gmn + 5.0 g CA(Reference) xxxx xxxx xxxx xxxxxxxx xxxx 2 24 mg Mg + 4.0 g gmn + 5.0 g CA 142.7 92.9 13.3 xxxx xxxxxxxx 3 42 mg Mg + 4.0 g gmn + 5.0 g CA 146.0 106.2 19.9 xxxx xxxx xxxx 463 mg Mg + 4.0 g gmn + 5.0 g CA 152.6 96.2 29.9 xxxx xxxx xxxx 5 207 mgMg + 4.0 g gmn + 5.0 g CA 195.8 192.4 175.9 179.2 165.9 132.7  6 0.1 gMg + 4.0 g gmn 116.1 126.1 0.0 xxxx xxxx xxxx 7 0.1 g Mg + 4.0 g gmn +0.5 g CA 139.4 142.7 0.0 xxxx xxxx xxxx 8 0.1 g Mg + 4.0 g gmn + 1.0 gCA 149.3 149.3 145.6 132.7  89.6  68.00 9 0.1 g Mg + 4.0 g gmn + 2.0 gCA 152.6 152.6 132.7 102.9  86.3 64.7 10 0.1 g Mg + 4.0 g gmn + 4.0 g CA169.2 149.3 132.7 116.1 109.5 97.9 BGV BGV BGV BGV BGV Formulas/100 mLDW 285-Hr. 321-Hr. 492-Hr. 696-Hr. 936-Hr. 1 4.0 g gmn + 5.0 gCA(Reference) xxxx xxxx xxxx xxxx xxxx 2 24 mg Mg + 4.0 g gmn + 5.0 g CAxxxx xxxx xxxx xxxx xxxx 3 42 mg Mg + 4.0 g gmn + 5.0 g CA xxxx xxxxxxxx xxxx xxxx 4 63 mg Mg + 4.0 g gmn + 5.0 g CA xxxx xxxx xxxx xxxxxxxx 5 207 mg Mg + 4.0 g gmn + 5.0 g CA 43.1 xxxx xxxx xxxx xxxx 6 0.1 gMg + 4.0 g gmn xxxx xxxx xxxx xxxx xxxx 7 0.1 g Mg + 4.0 g gmn + 0.5 gCA xxxx xxxx xxxx xxxx xxxx 8 0.1 g Mg + 4.0 g gmn + 1.0 g CA  0.0 xxxxxxxx xxxx xxxx 9 0.1 g Mg + 4.0 g gmn + 2.0 g CA  0.0 xxxx xxxx xxxxxxxx 10 0.1 g Mg + 4.0 g gmn + 4.0 g CA 96.2 96.2 76.3 56.4 59.7Abbreviations: BGV—Bubble Gel Volume; gmn—glucomannan; DW—distilledwater; CA—citric acid; mL—milliliters; Tot.—Total; mg—milligrams;Hr.—Hour; Mg—magnesium metal powder

TABLE 4 Time Course of Molecular Hydrogen (H₂) Generation in MagnesiumMetal Powder (Mg) - Glucomannan H₂ Gels with Antioxidants and Acids 1hour 1 hour 1 hour 6 hour 6 hour 6 hour Gel Gel Bubble Gas Gel BubbleGas Powder Formulas mixed with Wt. Dens. Vol. Vol. Vol. Vol. Vol. Vol.Row 100 mL Distilled Water (DW) (g) g/mL (mL) (mL) (mL) (mL) (mL) (mL) 10.5 g ascorbic acid + 4 g gmn. 101.8 0.852 119.5 xxxxxx xxxxxx 119.5xxxxxx xxxxxx 2 0.1 g Mg. + 0.5 g ascorbic acid + 4 g gmn. 102.3 0.752136.0 136.0 16.5 156.0 156.0 36.5 3 0.5 g Na ascorbate + 0.5 g Kcitrate + 4 g gmn. 102.5 0.870 119.5 xxxxxx xxxxxx 116.1 xxxxxx xxxxxx 40.1 g Mg + 0.5 g Na ascorbate + 0.5 g 102.2 0.751 136.0 136.0 16.5 152.6152.6 36.5 K citrate + 4 g gmn. 5 0.5 g isoascorbic acid + 4 g gmn.102.1 0.867 119.5 xxxxxx xxxxxx 112.8 xxxxxx xxxxxx 6 0.1 g Mg + 0.5 gisoascorbic acid + 4 g gmn. 101.8 0.731 139.4 139.4 19.9 142.7 142.729.9 7 0.5 g Na ascorbate + 4 g gmn. 101.9 0.853 119.5 xxxxxx xxxxxx119.5 xxxxxx xxxxxx 8 0.1 g Mg + 0.5 g Na ascorbate + 4 g gmn. 102.30.856 119.5 119.5  0.0 129.4 129.4  9.9 9 0.5 g salicylic acid + 4 ggmn. 101.6 0.862 119.5 xxxxxx xxxxxx 117.8 xxxxxx xxxxxx 10 0.1 g Mg +0.5 g salicylic acid + 4 g gmn. 101.9 0.660 154.3 154.3 34.8 152.6 152.634.8 11 0.5 g Na bisulfite + 4 g gmn. 102.2 0.856 119.5 xxxxxx xxxxxx116.1 xxxxxx xxxxxx 12 0.1 g + 0.5 g Na bisulfite + 4 g gmn. 102.2 0.655156.00  156.00 36.5 152.6 152.6 36.5 Abbreviations: gmn—glucomannan;DW—distilled water; Mg—magnesium metal powder; Dens.—density;mL—milliliters; H₂—molecular hydrogen; mg—milligrams; K—Potassium;Na—sodium; Vol.—volume

As listed in Table 4, powders were prepared from 0 to 0.1 gram magnesiummetal powder, 4 grams of glucomannan and 0.5 grams of ascorbic acid or0.5 grams of sodium ascorbate plus 0.5 grams of potassium citrate or 0.5grams of isoascorbic acid or 0.5 grams of salicylic acid or 0.5 grams ofsodium bisulfite.

Gels were prepared, at 22 -25 degrees centigrade, by taring the powdersinto empty 239 mL Arrowhead® water bottles, then adding 100 mL ofdistilled water (DW), mixing vigorously by shaking until the gel formedas indicated by perception of increased viscosity. Gels start to form15-30 seconds after starting to mix the formulas with water. The bottleswere then tightly capped.

After allowing the gels to settle, the total weights of the gel plus theweight of the bottle were gravimetrically determined. Bottles were foundto weigh 10.3 grams. Thus, the weight of the gels was determined bysubtracting the weight of a bottle from the total weight of the gel plusthe bottle. The volume of the gels was calculated based upon the factthat the Arrowhead® bottle volume in contact with the gel is a cylinder.The measurement of the volume of a cylinder is the height of the gel, incentimeters (cm.) times the area of the base of the bottle that wasdetermined to be 33.18 square cm. The height of the gels was measuredwith a 0.05 cm. graduated ruler. The density of the gels was determinedby dividing the weight of the gel by its calculated volume.

Bubbly gel volumes (BGV) were determined by measuring the length (gelheight) of the bubbly gel and multiplying by the 33.18 sq. cm. area.

The volume occupied by molecular hydrogen is calculated by subtractingthe BGV from the control gel volume that does not contain magnesiummetal powder, i.e., those control gels that do not generate molecularhydrogen as indicated as “Reference” in Table 2.

IX. DEFINITIONS

Unless defined otherwise, all terms of art, notations and othertechnical and scientific terms or terminology used herein are intendedto have the same meaning as is commonly understood by one of ordinaryskill in the art to which the claimed subject matter pertains. In somecases, terms with commonly understood meanings are defined herein forclarity and/or for ready reference, and the inclusion of suchdefinitions herein should not necessarily be construed to represent asubstantial difference over what is generally understood in the art.

Throughout this application, various embodiments may be presented in arange format. It should be understood that the description in rangeformat is merely for convenience and brevity and should not be construedas an inflexible limitation on the scope of the disclosure. Accordingly,the description of a range should be considered to have specificallydisclosed all the possible subranges as well as individual numericalvalues within that range. For example, description of a range such asfrom 1 to 6 should be considered to have specifically disclosedsubranges such as from 1 to 3, from 1 to 4, from 1 to 5, from 2 to 4,from 2 to 6, from 3 to 6 etc., as well as individual numbers within thatrange, for example, 1, 2, 3, 4, 5, and 6. This applies regardless of thebreadth of the range.

As used in the specification and claims, the singular forms “a,” “an,”and “the” include plural references unless the context clearly dictatesotherwise. For example, the term “a sample” includes a plurality ofsamples, including mixtures thereof

The terms “determining,” “measuring,” “evaluating,” “assessing,”“assaying,” and “analyzing” are often used interchangeably herein torefer to forms of measurement. The terms include determining if anelement is present or not (for example, detection). These terms caninclude quantitative, qualitative or quantitative and qualitativedeterminations. Assessing can be relative or absolute. “Detecting thepresence of” can include determining the amount of something present inaddition to determining whether it is present or absent depending on thecontext.

The terms “subject,” “individual,” or “patient” are often usedinterchangeably herein. A “subject” can be a biological entitycontaining expressed genetic materials. The biological entity can be aplant, animal, or microorganism, including, for example, bacteria,viruses, fungi, and protozoa. The subject can be tissues, cells andtheir progeny of a biological entity obtained in vivo or cultured invitro. The subject can be a mammal. The mammal can be a human. Thesubject may be diagnosed or suspected of being at high risk for adisease. In some cases, the subject is not necessarily diagnosed orsuspected of being at high risk for the disease.

The term “in vivo” is used to describe an event that takes place in asubject's body.

The term “ex vivo” is used to describe an event that takes place outsideof a subject's body. An ex vivo assay is not performed on a subject.Rather, it is performed upon a sample separate from a subject. Anexample of an ex vivo assay performed on a sample is an “in vitro”assay.

The term “in vitro” is used to describe an event that takes placescontained in a container for holding laboratory reagent such that it isseparated from the biological source from which the material isobtained. In vitro assays can encompass cell-based assays in whichliving or dead cells are employed. In vitro assays can also encompass acell-free assay in which no intact cells are employed.

As used herein, the term “about” a number refers to that number plus orminus 10% of that number. The term “about” a range refers to that rangeminus 10% of its lowest value and plus 10% of its greatest value.

As used herein, the terms “treatment” or “treating” are used inreference to a pharmaceutical or other intervention regimen forobtaining beneficial or desired results in the recipient. Beneficial ordesired results include but are not limited to a therapeutic benefitand/or a prophylactic benefit. A therapeutic benefit may refer toeradication or amelioration of symptoms or of an underlying disorderbeing treated. Also, a therapeutic benefit can be achieved with theeradication or amelioration of one or more of the physiological symptomsassociated with the underlying disorder such that an improvement isobserved in the subject, notwithstanding that the subject may still beafflicted with the underlying disorder. A prophylactic effect includesdelaying, preventing, or eliminating the appearance of a disease orcondition, delaying or eliminating the onset of symptoms of a disease orcondition, slowing, halting, or reversing the progression of a diseaseor condition, or any combination thereof. For prophylactic benefit, asubject at risk of developing a particular disease, or to a subjectreporting one or more of the physiological symptoms of a disease mayundergo treatment, even though a diagnosis of this disease may not havebeen made.

The term “probiotic” means live microorganisms intended to providehealth benefits when consumed, generally by improving or restoring thegut flora.

The term “prebiotic” means compounds in food that induce the growth oractivity of beneficial microorganisms such as bacteria and fungi.

The term “sustainability” is defined herein as the ability to hold H₂ ingels or solutions over the short—term.

The term “stability” is defined as the ability to hold H₂ in a gel overthe longer-term, i.e., longer than 24 hours.

The section headings used herein are for organizational purposes onlyand are not to be construed as limiting the subject matter described.

X. SPECIFIC EMBODIMENTS

Certain specific embodiments are envisioned which include:

1. A glucomannan solution comprising a concentration of glucomannan andhydrogen (H₂), comprising an organic acid, wherein the organic acid isselected from the list consisting of citric acid, malic acid, lacticacid, acetic acid, tartaric acid, succinic acid, phosphoric acid or anycombination thereof.

2. The solution of claim 1, wherein the hydrogen (H₂) is present at aconcentration of greater than about 100 ppb (parts per billion) hydrogen(H₂).

3. The solution of claim 1, wherein the volume of the glucomannansolution comprising a concentration of glucomannan and hydrogen (H₂) isat least 0.01%, at least 0.1%, at least 1%, at least 10%, or at least20% greater than the volume of a corresponding glucomannan solutionwhich does not comprise H₂.

4. The solution of claim 1, wherein upon exposure to standardtemperature and pressure (STP) for 240 minutes, the H₂ concentration isat least about 70% of the initial H₂ concentration as measured in partsper billion (ppb).

5. The solution of claim 1, wherein the glucomannan concentration isfrom about 0.00001% to about 7.5%.

6. The solution of claim 1, wherein the solution is a gel.

7. The solution of claim 1, wherein the solution is a flowable liquid.

8. The solution of claim 1, wherein the H₂ is present in a gaseous form.

9. The solution of claim 1, wherein, upon exposure of the glucomannansolution to standard temperature and pressure (STP) for 240 minutes, theconcentration of hydrogen in the glucomannan solution declines by lessthan 1%, less than 5%, less than 10%, less than 15%, less than 20%, lessthan 25%, or less than 30%. as measured in parts per billion (ppb).

10. The solution of claim 9, wherein, upon exposure of the glucomannansolution to standard temperature and pressure (STP) for 240 minutes, theconcentration of hydrogen in the glucomannan solution is at least 70% ofthe H₂ concentration in the solution prior to the exposure as measuredin parts per billion (ppb).

11. The solution of claim 1, further comprising a base metal.

12. The solution of claim 11, wherein the base metal is selected fromthe group consisting of lithium, potassium, strontium, calcium, sodium,magnesium metal powder, aluminum, zinc, chromium, manganese, iron, andany combination thereof

13. The solution of claim 12, wherein the base metal is magnesium metalpowder.

14. The solution of claim 13, wherein the magnesium metal powder ispresent in the glucomannan solution in an amount from about 0.00001% w/vto about 2% w/v.

15. The solution of claim 1, wherein the citric acid is present in anamount from about 0.1% w/v to about 15% w/v.

16. The solution of claim 1, wherein the malic acid is present in anamount from about 1% (w/v) to about 50% w/v.

17. The solution of claim 1, wherein the lactic acid is present in anamount from about 1% w/v to about 10% w/v.

18. The solution of claim 1, further comprising an aqueous solvent.

19. An H₂-generating composition comprising:

lactic acid;

glucomannan;

magnesium metal powder;

glycerin; and

an aqueous solvent.

20. The composition of claim 19, wherein the composition is a cream,gel, foam, ointment, lotion, or liquid.

21. The composition of claim 19, wherein the composition is adapted forapplication to the skin of a subject.

22. The composition of claim 21, wherein the composition provides amoisturizing effect to the skin of the subject.

23. A bandage comprising the composition of claim 21.

XI. EXAMPLES

The following examples are included for illustrative purposes only andare not intended to limit the scope of the invention.

Example 1: Effect on Molecular Hydrogen Content of Varying GelComponents

1. Gel Preparation

The gel formulations presented in Table 2 were prepared by first placingthe glucomannan, magnesium metal and/or citric acid powders in 8-ounceplastic cups. Then, 100 mL of distilled water was added. Contents mixedby hand with a utensil, until the gel started to form—in less than twominutes.

2. Effects of Varying Magnesium Metal Powder

The results presented in Table 2 show the effects on gel parameters ofvarying the components of the gels. The results presented in Rows 1 to 6show the effect varying the magnesium metal powder concentration (Mg) onGel Density (Column 3), and molecular hydrogen (H₂) volume in the gel(Column 4). H₂ volume in the gel is calculated by subtracting the volumeof the control gel, without Mg (see Row 1) from the gels containing 11to 207 mg magnesium metal powder (Mg). For example, in Column 6, the gelvolume of the control gel in Row 1 is subtracted from the test gelvolume seen in Row 2; again, the gel volume of the control gel in Row 1is subtracted from the test gel volume in Row 3, etc.

The results indicate that H₂ in the gel increases with the amount of Mgin the formulation (Column 4). Analysis of the results in Column 5indicates that the H₂ per milligram of Mg in the formulations decreasesas the concentration of Mg increases in the gel. Thus, the efficiency ofH₂ generation or capture of H₂/mg of Mg in the gel decreases withincreasing Mg in the formulation. Observation indicates that for theH₂-generating gels, bubbles were evenly dispersed from bottom to top ofthe gels affecting a uniform perception of bubble porosity. Bubbles arenot seen in the control gel (Row 1).

3. Effects of Varying Citric Acid

The results presented in Rows 7-18 of Table 2 demonstrate the effect ofvarying the concentration of citric acid (CA) on gel density andmolecular hydrogen (H₂) retention in the gel. The odd numbers are thecontrol gels—without magnesium metal powder (Mg). The control geldensity is always greater than that of the experimental gels. The H₂ inthe gels is calculated by subtracting the odd numbers (i.e., controls)from the even number formulations, as described above. Analysis of theresults indicate that H₂ in the gel increases with the amount of citricacid in the formulation. Analysis of the results in Column 5 indicatesthat the H₂ per milligram of citric acid in the formulation decreases asthe concentration of citric acid increases in the gel. Thus, theefficiency of generation of H₂ in the gel decreases with increasingcitric acid in the formulation.

4. Effects of Varying Glucomannan

The results presented in Rows 19-34 of Table 2 show the effect ofvarying the concentration of glucomannan (gmn) on gel density and H₂ inthe gel. The odd numbers are the control gels—without Mg. Density in thecontrol gels is always greater than that of the experimental gels. TheH₂ in the gels in calculated by subtracting the odd numbers (controls)from the even number formulations. Analysis of the results indicate thatthe H₂ calculated to be in the gel does not always increase with anincreasing amount of glucomannan in the formulation. At the lowest doseof gmn tested—as indicated in Rows 19 and 20, the Bubble Gel Volume(BGV) shown in Column 7, is markedly less than the Total Gel Volume(Column 6)—indicating a lesser ability of the lowest concentration ofgmn to generate H₂ or to hold H₂ within the gel. In contrast, for higherconcentrations of gmn (Rows 22, 24, 26, 28, 30, 32, 34) the Bubble GelVolume (BGV)(Column 7) is equal to the Total Gel Volume (Column 6). The2- and 3-gram/100 mL glucomannan gels appear to hold less H₂ than the1-gram/100 mL glucomannan gel. This appears to be an artifact due totheir control gels having a larger Total Gel Volume. However, as will beshown, below, gels with a higher concentration of glucomannan hold H₂for a longer period of time.

5. Discussion of the Results in Table 2

Analysis of the results in Table 2 indicate that increasing theconcentration of magnesium metal powder (Mg) and citric acid (CA) in thegel formulations increases the amount of molecular hydrogen (H₂) in thegel while decreasing the efficiency of generation and/or capture of H₂in the gel. Citric acid is known to have a strong effect on removal ofthe passivation coat of magnesium oxide from magnesium metal (See, Uan,J-Y. et. al.(2009) J. of Hydrogen Energy 34 (15), 6137-6142). Alteringthe concentration of gmn in the gels presents a more complex H₂response. The complex interactions between Mg, water, gmn, and citricacid regarding gel density may help to explain this anomalous behavior.

The information presented in Table 2 may be used in designing gels fordifferent purposes. For example, one application may require fast, largevolume release of H₂ from the gel. If so, a low concentration of gmn(e.g., 0.5-1 g/100 mL) and high concentrations of Mg (60-200 mg/100 mL)and an acidic pH would be suggested.

Cost of generating gels, particularly for a specific application, mustbe taken into consideration. The cost of magnesium metal powder andorganic acids are inexpensive, while the cost of glucomannan perkilogram is much more expensive.

Another important consideration for food applications is taste. Tastecan be modified by addition of excipients and functional agents to themagnesium metal powder-glucomannan gels.

Example 2: Effect of Exemplary Antioxidants and Acids on MolecularHydrogen (H₂) Generation in Aqueous Magnesium Metal Powder(Mg)-Glucomannan (gmn) Gels

Gel preparation was performed as described in Example 1. The results inTable 4 show the effect of incorporating exemplary antioxidants, saltsof antioxidants or exemplary acids on: aqueous magnesium metalpowder—glucomannan gel formation; gel density and the volume of H₂ inthe gels. Evaluations at one-hour and at six-hours after gel formationare shown.

For all but one gel formula, i.e., that containing 0.5 grams of sodiumascorbate, (See Table 4, Rows 7 and 8), densities of the control gels atthe 1-hour evaluation (Table 4, Rows 1, 3, 5, 9, 11) were higher, asfound for those gels tested versus the control gels as shown in Table 2.Thus, at the 1-hour evaluation, 0.5 g sodium ascorbate/100 mL DW in the0.1 magnesium metal powder - glucomannan gel does not produce an amountof H₂ that would lower the gel density. In contrast, at the 6-hourevaluation, it was found that 9.9 mL of H₂ was present in this gel.Thus, 0.5 g sodium ascorbate/100 mL DW in a magnesium metalpowder—glucomannan gel slowly produces gas that is retained in the gelover the 1 to 6-hour period. This slower process of H₂ generation mayhave an advantage in situations where gel formation takes place fasterthan H₂ generation. That is, a higher percentage of H₂ can besequestered in the gel.

Analyzing the 1 to 6-hour time course for H₂ generation in gelscontaining 0.5 g ascorbic acid (Table 4, Rows 1, 2); or 0.5 g sodiumascorbate plus 0.5 g of potassium citrate (Rows 3, 4); or 0.5 gisoascorbic acid (Rows 5, 6), it is observed that H₂ volume sustained inthe gel is between 16.5 and 19.9 mL at the one hour evaluation. It risesto between 29.9 and 36.5 mL at the 6-hour evaluation. Knowledge of thisslow generation and sequestration of H₂ in the gel is useful fortrapping the maximum amount of H₂ in the gel. That is, the gel can beformed before appreciable H₂ is generated and escapes to theenvironment. Once the gel is formed, the additional H₂ generated will betrapped for an extended period.

In contrast, magnesium metal powder—glucomannan gel containing either0.5 g salicylic acid or 0.5 g sodium bisulfate reach their maximum H₂volume in the gel at 1 hour post gel formation. Like citric and otherhydroxy acids, these acids affect fast generation of H₂ in the gels.

Example 3: Effect of Some Acids on the Generation of Molecular Hydrogenin Magnesium Metal Powder (Mg)-Glucomannan (gmn) Gels

The results shown in Table 5 demonstrate the effects of some organicacids and one inorganic acid on the generation of molecular hydrogen(H₂) in magnesium metal powder (Mg)-glucomannan (gmn) aqueous gels. Forthis set of results, dry 296 mL empty water bottles were used. The emptybottles, with caps, weigh 9.6 g. The weight of the gels was determinedby subtracting the weight of the empty bottle from the total weight. Thearea of the circumference of the bottle is 30.19 square cm (i.e., 6.2cm. diameter). Thus, volumes of the gels were calculated by 30.19 squarecm.-multiplied by the height of the gels, in cm.

TABLE 5 Effect of Acids on Generation of Molecular Hydrogen (H₂) inMagnesium Metal Powder (Mg) - Glucomannan (gmn) Gels Bubbly Tot Dens.Gas Gel Gel pH Row Test Formulas/100 mL DW g/mL mL (mL) mL unit 1 4.0 ggmn + 4 g lactic acid/DW 0.974 0 0.0 108.7 3.16 2 0.1 g Mg + 4.0 g gmn +4.0 g lactic acid/DW 0.762 30.2 138.9 138.9 3 4.0 g gmn + 4.0 g tartaricacid/DW 0.974 0 0.0 108.7 1.62 4 0.1 g Mg + 4.0 g gmn + 4.0 g tartaricacid/DW 0.712 33.2 141.9 141.9 5 4.0 g gmn + 4 g succinic acid/DW 1.0270 0.0 102.7 2.14 6 0.1 g Mg + 4.0 g gmn + 4.0 g succinic acid/DW 0.74439.2 141.9 141.9 7 4.0 g gmn + 4.8 mL 85% phosphoric acid/DW 1.088 0 0.096.6 0.98 8 0.1 g Mg + 4.0 g gmn + 4.8 mL 85% phosphoric 0.880 24.2120.8 120.8 acid/DW 9 4.0 g gmn + 4.0 g malic acid/DW 0.997 0 0.0 105.71.81 10 0.1 g Mg + 4.0 g gmn + 40 g malic acid/DW 0.712 42.2 147.9 147.911 0.1 g Mg + 4.0 g gmn + 4.0 g malic acid/LVVWD 0.730 39.6 144.9 144.912 0.1 g Mg + 4.0 g gmn + 4.0 g malic acid/ROW 0.751 34.7 140.4 140.4 130.1 g Mg + 4.0 g gmn + 4.0 g malic acid/SW 0.752 34.7 140.4 140.4Abbreviations: gmn—glucomannan; DW—distilled water; SW—soft water;ROW—Reverse Osmosis Water; LVVWD—Las Vegas City Water; Tot.—Total;H₂—molecular hydrogen; Mg—magnesium metal powder; g—grams;Dens.—density; mL—milliliters.

The results in Columns 3 and 4, respectively, show the effects on geldensity and H₂ gas volume due to incubating the different acids, mixedinto magnesium metal powder-glucomannan gel powders, and then mixed withwater. The odd numbered formulations 1, 3, 5, 7 and 9 arecontrols—without Mg. The even numbered gels, as well as 11, 12 and 13each contain 0.1 g of Mg.

The results listed in Column 3 of Table 5 show clearly that thedensities of the gels generated with Mg present in the gel, have muchlower densities relative to their controls—without Mg present. Thislowering of the density is due to the presence of large numbers of H₂bubbles and dissolved H₂-in the gel.

Column 4 of Table 5 lists the volume of H₂ gas that is present in eachgel. The volumes of H₂ are based upon the difference in the volume ofthe Mg containing gels and their controls without Mg (Rows 1, 3, 5, 7and 9). The volume of H₂ in the gels range from 24.2 mL for thephosphoric acid containing gel to 42.2 mL for the malic acid containinggel generated with distilled water. Although all types of water used forpreparing magnesium metal powder-glucomannan gels readily generates H₂,use of distilled water appears to be the most effective at generating H₂(See Rows 10-13).

Thus, all the acids tested affect the content of H₂ in the gels andexpansion of the volume of gels. The difference in the amount of H₂ inthe gels depends on the nature of the acid, the concentration thereof,and the pH of the composition. Comparing the H₂ in the gels shown inTable 5 with that generated by a comparable amount of citric acid, (SeeTable 2, Row 16) citric acid is a more potent effector of H₂ in theMg-glucomannan gels.

Example 4: Room Temperature Stability of Molecular Hydrogen (H₂) inMagnesium Metal Powder (Mg)-glucomannan (gmn) Gels

Longer term studies were carried out to determine the time course ofloss of H₂ from magnesium metal powder-glucomannan gels. Here, we definesustainability as the ability to hold H₂ in gels or solutions over theshort-term. We define stability as the ability to hold H₂ in the gelsover the longer-term, i.e., longer than 24 hours.

Stability of molecular hydrogen (H₂) in the magnesium metalpowder-glucomannan gels is estimated by measuring the extent that aparticular gel will maintain its bubble gel volume (BGV)—over time.

For this Stability Study, some of the test samples shown in Table 2 werestudied for up to 936 hours (39 days). Comparing the results in Rows 1-5of Table 3, it is seen that as the concentration of Mg in the gels isincreased, the longer the visible bubbles (BGV) last in the gels.Comparing the rate of drop of the BGV, it appears that the highestconcentration of Mg (207 mg) is more effective at maintaining H₂ bubblesin the gel. That is, by 108 hours of stability testing, the gelscontaining respectively, 24, 42, and 63 mg of Mg have lost,respectively, 91.0, 86.4, and 80.4% of their bubble gel volume. Incontrast, the gel containing 207 mg of Mg lost only 10.2% of its bubblygel volume (BGV). The gel containing 207 mg Mg maintained 68% of its BGVup to 261 hours (10.9 days) - after gel preparation. Thus, there may bea synergistic effect of Mg in maintaining BGV in glucomannanformulations. It is possible that an interaction of Mg and/or magnesiumhydroxide takes place with the H₂ bubble complex in the glucomannan gel.Also, an interaction of Mg particles with H₂ microbubbles in the gel,would tend to keep the H₂ bubbles from escaping from the gel.

Comparing the results in Rows 6-10 of Table 3, it is seen that as theconcentration of citric acid increases, the stability of H₂ bubbles inthe gel (BGV) increases. Thus, it has been unexpectedly found thatcitric acid increases the stability of H₂ in aqueous Mg-glucomannanformulations.

Example 5: Refrigerated Study of Molecular Hydrogen (H₂) Stability inAqueous Magnesium Metal Powder-Glucomannan Gels

1. Experimental

A study was carried out to determine the stability of H₂ in a magnesiummetal powder-glucomannan gel under refrigerated conditions (1-4 deg.C.). A batch consisting of 1.1 g of crude magnesium metal powder (Mg),44.0 g of Best Naturals® konjac glucomannan powder and 5.5 g of citricacid was prepared and mixed thoroughly. Aliquots of 9.1 g of the batchof powder were added to 5 empty 237 mL plastic bottles. Thereafter, 100mL of distilled water was added to each bottle. The bottles were tightlycapped and shaken vigorously while the gels formed. Bottles labeled#6-10 were designated for the refrigerated stability study. After thegels formed, a line was drawn on the bottle where the gel—air interfaceformed, thereby delineating the height of the gel. Knowing the area ofthe base of the bottle as 33.18 square cm, the volume of the gels wascalculated, i.e., from the volume of a cylinder. Initially, the entirevolume of the gels contained numerous bubbles, of diverse sizes—from topto bottom of the bottle. The volume of gel containing bubbles wasdesignated as the Bubble Gel Volume (BGV). It was observed that thebubbles diffused up from the bottom of the gel with the passage of time.It is observed that the gels become depleted of H₂ bubbles-frombottom-to-top of the gel, as time passes. The change in the BGV, withtime, was determined by measuring the length of the gel that stillcontained bubbles and multiplying times the circumference of the bottleto obtain the remaining BGV. To gain access to the gel at completion ofthe time course of the experiment, the top section of the plastic bottlewas cut off exposing the gel for measurements of dissolved H₂. DissolvedH₂, in the gels, was measured with the Trustlex® Molecular Hydrogen (H₂)meter, without the guard that protects the electrode. The guard isremoved since it would deny access of the Trustlex® electrode to thegel.

2. Results

The time course of results is shown in Table 6. As shown in Column 2,there is a progressive, slow reduction in BGV—with time. At Day 73, thelast day of the Study, the gel retained 51.1% of the baseline BGV. H₂measurements, at that time, indicated that there was 250 ppb dissolvedH₂ in the Gel.

TABLE 6 Refrigerated (1-4 C.) Study on the Stability of MolecularHydrogen in a Magnesium Metal Powder - Glucomannan Gel Dissolved %Change H₂ Day BGV in BGV ppb 0 169.3 xxxx NM 2 163.9 −3.2 NM 13 148.7−9.1 NM 29 148.7 −9.1 432 41 132.7 −21.6 459 50 119.5 −29.4 400 62 124.5−26.5 379 73 86.6 −48.9 250 Abbreviations BGV—Bubble Gel Volumeppb—parts per billion molecular hydrogen (H₂) NM—Not measured

This remarkable retention of H₂ in the Mg-gmn gel was unexpected. H₂ isthe universe's smallest molecule and it is thought to be able to rapidlydiffuse through most materials. A plastic container should not provide along-term barrier to H₂ diffusion. Rather, there is a stabilization ofboth H₂ in bubbles and dissolved H₂ in the magnesium metalpowder-glucomannan gel.

There are interesting applications of longer term, low temperature,storage of H₂ gels. For example, there are applications in therefrigerated food category. H₂-rich, Mg-gmn viscous solutions and gelscan be formulated into various food products—including gels. Suchproducts could be manufactured and stored, for extended periods of time,by manufacturers or consumers.

Example 6: Some Special Properties of Magnesium Metal Powder-GlucomannanComplexes

1. Molecular Hydrogen, but not Carbon Dioxide is Retained in GlucomannanGels

a. Introduction

A study was carried out to compare the effects of potassiumbicarbonate—which generates carbon dioxide gas (CO₂) in acidicsolutions, and magnesium metal powder—which generates molecular hydrogen(H₂) in acidic solution—on glucomannan gel volume. The ‘000’ capsulescontaining the ingredients were immersed in aqueous 1.25% acetic derivedfrom vinegar in sealed bottles. This study was done: 1) to determine ifthe effect of H₂ on increasing gel volume is unique to use of ahydrogen-generating system; 2) to determine the effects on these gasproducing agents on both gel volume and headspace volume in a closedsystem; 3) to have the closed system serve as a model for gel behaviorin the upper gastrointestinal tract; 4) to determine the effect ofincreasing concentrations of glucomannan on gel volume expansion.

b. Experimental

Formulations, as listed in Table 1, were prepared by mixing the powderingredients and then manually filling vegetarian “000” Vcaps® capsulesobtained by Cap-M-Quik.com. Different numbers of capsules were used toaccommodate the volume of each powder formulation (See Column 9 of Table1). Diluted vinegar (1.25% acetic acid), in separate 2500 mL lots, wasprepared by mixing 625 mL white vinegar (5% acetic acid) with 1875 mL ofdistilled water (DW). Great Value® purified water bottles were emptiedand dried before use. When these bottles are filled and topped off, theyhold 540 mL of liquid.

Both magnesium metal powder (Mg)-glucomannan capsules, and potassiumbicarbonate-glucomannan capsules were tared before being added to theempty bottles. The weight of the empty capsules was accounted for.Thereafter, the bottles were ‘topped off’ with the 1.25% acetic acidsolution and tightly capped. The time of starting the experiment wasrecorded. The contents were periodically mixed by rotating the bottlesby hand. Experiments were carried out at 23 C.

H₂ Blue®, a methylene blue-platinum catalyst titration method, used asinstructed by the manufacturer (H₂ Sciences.com), was employed toestimate dissolved H₂ in ppm. One drop of test solution is equivalent to0.1 ppm H₂. For example, if it takes 5 drops of the test solution toturn six mL of a solution blue, then the solution contains 0.5 ppm H₂.Testing was performed in a 20 mL graduated plastic vial. The pHmeasurements were taken with an EXTECH® ExStik® PH100 pH meter that wasperiodically calibrated.

Generation of H₂ gas from magnesium metal powder reacting with dilutevinegar and generation of carbon dioxide (CO₂), from potassiumbicarbonate reacting with dilute vinegar, in the sealed bottles createsa headspace. The volume of the 1.25% acetic acid liquid displaced by thegases generating the headspace in the bottles was measured as follows:At completion of the study, there was a displacement of liquid on thetop of the sealed bottles, i.e., the headspace. A marker pen was thenused to delineate the length and circumference of the headspace. Themarker pen was also used to delineate the length and circumference ofthe gel in each bottle. After emptying and rinsing the bottles, leavingthe caps in place, a scissors was used to ‘cut out’ and save the plasticsection of the bottle representing the headspace plus the plasticsection of the bottle previously containing the gel. The bottle capremained in place as a base to retain liquid in the upper portion of the‘cut out’ section of the bottle. A gravimetric procedure was used todetermine the amount of solution in the ‘cut out’ section of the bottle.That is, after weighing the empty plastic piece representing theheadspace plus the gel, distilled water was added to the plastic sectionrepresenting the headspace unit plus the gel—until water totally filledthe headspace container. Water contained in the section representing theheadspace was weighed and recorded. The upper plastic sectionrepresenting the headspace was then cut away leaving the sectionrepresenting the gel. The same gravimetric procedure was used todetermine the volume occupied by the gel.

c. Results

Table 1, Rows 1-15, displays the 15 formulations tested. The capsuleswere placed in the plastic bottles, topped off with 540 mL of the 1.25%acetic acid solution and capped tightly. Incubation time was 5 hours. Itshould be noted that the 000 capsules readily dissolve in the aqueous1.25% acidic acid solution.

Effect of Potassium Bicarbonate

The result in Row 1 of Table 1 shows that addition of the capsulecontaining 0.1 g Mg, without glucomannan, does not result in gelformation—as expected. However, it generates H₂ gas pressure therebycreating a 37.6 mL of headspace. It also produces 0.7 ppm of molecularhydrogen (H₂) that is dissolved in the 1.25% acetic acid solution. Thus,in this system, H₂ can exist in both the headspace and be dissolved inthe aqueous acidic solution.

The results in Rows 2-5 of Table 1 show formulations containing 2 gramsof glucomannan (gmn) and different concentrations of potassiumbicarbonate—which generates carbon dioxide (CO₂) in this acidicsolution. Potassium bicarbonate was tested with glucomannan to determineif the resultant generation of CO₂ could alter gel formation and affectgel expansion. The results show that incubating theglucomannan-containing formulations with increasing doses of potassiumbicarbonate, generates a head space of 0.0-14.3 mL in a dose-responsemanner (See Rows 2-5, Column 4). In contrast, a 1.6 g glucomannanformulation, without CO₂- producing potassium bicarbonate, does notproduce a head space (See Row 6 of Table 1). The total volume i.e., headspace plus gel volume affected by potassium bicarbonate (Rows 2-5,Column 5), is 13.4-30.9 mL. The gels alone, containing potassiumbicarbonate, range from 11.0 to 21.6 mL—where gel volume does notincrease with potassium bicarbonate content. Column 8 lists theefficiency of gel formation, i.e., the volume of gel produced per gramof glucomannan. The efficiency of this group ranges from 5.5 to 10.8 mLof gel per gram of glucomannan. There is a lack of a dose-responserelationship in affecting gel volume per gram of glucomannan—when testedwith potassium bicarbonate. The concentration of potassium bicarbonatein the gel (See Rows 2-5, Column 3 and 8) is not related to the volumeof gel formation. The formulation containing 1.6 g of glucomannan (Row6, Column 2), without potassium bicarbonate, is slightly more efficientat gel formation than the glucomannan gels that contain potassiumbicarbonate. (Rows 2-5, Column 8). Therefore, potassium bicarbonate and,in turn, CO₂ does not expand glucomannan gels. These observations onglucomannan-potassium bicarbonate compositions in aqueous acidicenvironments supports the hypothesis that there is a strong interactionbetween H₂ generation from magnesium metal powder and glucomannanresulting in the expansion of glucomannan gels that is a unique propertyof generating H₂ in glucomannan solutions and gels. That is, generationof any gas in aqueous-glucomannan gels will not expand the gel volume—asfound for H₂.

d. Effect of Magnesium Metal Powder

The results in Rows 7-15, Column 2 of Table 1 show magnesium metalpowder-glucomannan (Mg-gmn) formulations, in 000 capsules. Thesecapsules were added to 1.25% acetic acid, as a stomach acid model, asdiscussed above. Magnesium metal powder was combined with glucomannan,in capsules, to determine its effect on gel formation as well as todetermine the generation of molecular hydrogen (H₂) in this aqueousacidic solution. The results in Column 4 show that glucomannanformulations containing magnesium metal powder (Mg) generate a headspace of between 14.2 and 39.4 mL. The formulation that generates the14.2 mL headspace contains the lowest concentration of Mg (0.05 g) whilethe formulation that generates the largest head space contains both Mg(0.1 g) and potassium bicarbonate (0.8 g). Thus, both Mg and potassiumbicarbonate contribute to the head space volume. The gels produced bythe Mg containing glucomannan formulations range from 17.6-132.7 mL(Column 4). Increasing both magnesium metal powder and glucomannan leadsto increased gel volume. The efficiency of gel formation is inverselyrelated to the glucomannan concentration, where the lowest concentrationof gmn (0.2 g), in the presence of 0.1 g Mg, generates the most gel/gramof glucomannan. It is of interest that addition of 0.8 g potassiumbicarbonate reduces the efficiency of generation of gel volume bymagnesium metal powder (Row 7). This shows that the reaction ofmagnesium metal powder with water in the glucomannan—1.25% acetic acidsolution generates an expanded gel volume larger than would beanticipated from previous results. This generation of expanded gelvolume involves the sequestering of bubbly molecular hydrogen in the geland the presence of dissolved molecular hydrogen in the gel.

e. Removal of the Passivation of Magnesium Metal Powder by Glucomannan

Comparing the results in Row 6 of Table 1 with those of Rows 11-15 ofTable 1, it is seen that the increasing concentration of glucomannanincreases gel volume (Column 3) in a dose—response manner. Since, asshown in Row 6, without magnesium metal powder, the highestconcentration of glucomannan studied, i.e., 1.6 g, has a gel volume of18.8 mL (See Row 6, Column 3). Comparing this volume to the 73.4 mL gelvolume generated by the 1.6 g glucomannan plus 0.1 g magnesium metalpowder, the effect on generation molecular hydrogen in the gel isobvious. Thus, the generation of H₂ by 0.1 g magnesium metal powder inthe glucomannan gel has an effect of increasing gel volume by 390%.Further, comparing the results in Rows 1-15 of Table 1, it can be seenthat there is a dose-response relationship in increasing gel volume byincreasing the concentration of glucomannan. This effect must be due toincreasing molecular hydrogen in the gel, since all but one of theseformulations has much lower concentrations of glucomannan than thecontrol displayed in Row 6 of Table 1. These results point to a directinteraction between glucomannan and magnesium metal powder in theaqueous acidic solution—in promoting the generation of molecularhydrogen in the resultant gels. This interaction is best explained byglucomannan having the ability to catalyze the removal of the magnesiumoxide passivation coat from the surface of magnesium metal powderparticles.

Further, results shown here and in Table 14 and FIG. 1 demonstrate thatglucomannan, without citric acid, can affect the removal of thepassivation coat of magnesium oxide from magnesium metal powder.

f. Discussion

Generation of molecular hydrogen (H₂), in an acidic solution mimickingstomach acid, takes place when glucomannan is combined with magnesiummetal powder (Mg). This effect is observed by comparing the generationof 0.7 ppm H₂ by 0.1 g magnesium metal powder—without glucomannan (SeeRow 1, Table 1)—with the formulations containing 0.1 Mg with 0.2-4.0 gof glucomannan—which generates 0.8 to 1.5 ppm of dissolved molecularhydrogen (See Rows 7-15, Table 1).

There has been a failure of weight loss treatments and programs to stopthe progression of the obesity epidemic. Also, there is lack ofeffective and safe weight loss drugs. Obesity is only the ‘tip of theiceberg’. A newly uncovered inflammatory component of obesity is nowknown to lead to serious diseases, including Type 2 diabetes,cardiovascular disease, cancer, Alzheimer's disease, fatty liver diseaseand several autoimmune diseases. Thus, there is a need for a safe andeffective product that treats both the cause of obesity and theinflammatory component that affects the associated diseases—listedabove.

Molecular hydrogen (H₂)-generating magnesium metal powder(Mg)-glucomannan formulations delivered to the stomach by capsule,tablet or other pharmaceutical dosage forms, can create satiety bygenerating a feeling of fullness for 4-8 hours, while reducing obesityassociated inflammation due to the generation and sustained release ofanti-inflammatory molecular hydrogen.

Example 7: Effect of Ingestion of Magnesium Metal Powder(M₂)-Glucomannan (gmn) Capsules on Satiety

A subject experienced hunger sometime between early lunch (around 9:30AM) and dinner (around 5:30 PM). He would snack on ‘junk food’ beforedinner and found he was gaining unwanted weight.

It was suggested that when feeling hungry that he consumed a 7%magnesium metal powder-93% glucomannan powder mixture, encased incapsules where each capsule contained 0.4 grams powder per capsule.

In the first trial, he started feeling hungry at about 2:30 PM. He tookone 7% Mg-93% gmn capsule with an 8 oz. glass of water and was able toavoid snacking until 4:40 PM, upon which he ‘broke down’ and snacked.

In the second trial, he again started feeling hungry about 2:00 PM. Hetook three of the 7% Mg-93% gmn capsules with a 12 oz. glass of water.He was able to avoid snacking and ate his dinner on time. He did notexperience any adverse events from taking the 7% Mg-93% gmn capsules.

In the third trial, he again started feeling hungry about 2:00 PM. Hetook 6 of the 7% Mg-93% gmn capsules with about 15 oz. of water. Heexperienced a feeling of fullness within five minutes. He was able toavoid snacking. He could finish the main course of his dinner, butrefused desert, which he normally ate. The only side effect was afeeling of fullness. It did not alter his sleeping or bowel movementpatterns.

Example 8: Development of a Hydrogen-Rich, Low Calorie Lemon Gel

There is a need for a snack or desert that will substitute for highcalorie foods, provide a feeling of fullness—thereby supporting weightcontrol and fasting regimens.

A delicious tasting, 5 calorie lemon gel, retaining molecular hydrogen(H₂) and expanding in volume, thereby giving a feeling of fullness, wasthe objective of a product development program. Development took placeby a process of variation of the levels of magnesium metal powder (Mg)and glucomannan (gmn), along with testing D-L malic acid, ascorbic acid,iso-ascorbic acid and the natural sweetener-stevia, a natural lemonflavor powder (BioFinest®) and FDC Yellow #6. Several low-calorieversions of gels were prepared and tested for volume expansion of thegel due to H₂, sweetness, tartness, texture, color and lemon flavor. Theinitial formulation and taste testing studies which resulted in theelimination of some ingredients are not displayed here.

Table 7 displays the results of the last three sequential studiesinvolved in the process of development of the gel.

TABLE 7 Development of a Low Calorie, Hydrogen - Rich Lemon Gel BasedUpon Magnesium Metal Powder and Glucomannan 1-Hr Vol. Sweet- Tart- Tex-Inc. # Formulas/100 mL Distilled Water (DW) ness ness ture Comments (mL)Study 6218 1 8 mg Mg + 4.0 gmn + 0.8 g Stevia + 0.5 g 2 5 10 No LF, notsweet −5.6 LF + 0.3 g Na ascorbate 2 16 mg Mg + 4.0 gmn + 0.8 g Stevia +0.5 g 2 5 10 No LF, not sweet 5.6 LF + 0.3 g Na ascorbate 3 47 mg Mg +4.0 gmn + 0.9 g Stevia + 0.5 g 3 5 10 Better than 1 & 2 11.3 LF + 0.3 gNa ascorbate 4 79 mg Mg + 4.0 gmn + 0.7 g Stevia + 0.5 g 3 5 10 Same as3 14.4 LF + 0.3 g Na ascorbate 5 40 mg Mg + 4.0 gmn + 0.9 g Stevia + 0.7g 3 5 10 Little LF, not sweet 11.3 LF + 0.3 g Na ascorbate 6 39 mg Mg +4.0 gmn + 0.8 g Stevia + 1.0 g 3 4 10 Little LF, starchy 14.4 LF + 0.3 gNa ascorbate 7 38 mg Mg + 4.0 gmn + 0.8 g Stevia + 1.0 g 2 5 10 Bitter,not sweet 17.0 LF + 0.2 g isoascorbic acid 8 45 mg Mg + 4.0 gmn + 0.8 gStevia + 1.0 g 1 7 10 Bitter, not sweet 22.6 LF + 0.4 g isoascorbic acid9 41 mg Mg + 4.0 gmn + 0.8 g Stevia + 1.0 g 1 7 10 Bitter, not sweet11.3 LF + 0.2 g malic acid 10 43 mg Mg + 4.0 gmn + 0.8 g Stevia + 1.0 g4 7 10 Bitter, not sweet 19.8 LF + 0.4 g malic acid 11 44 mg Mg + 4.0gmn + 1.0 g Stevia + 1.0 g 3 4 10 No LF, not sweet 25.5 LF + 0.2 gascorbic acid 12 35 mg Mg + 4.0 gmn + 0.8 g Stevia + 1.0 g 2 7 10 No LF,not sweet 19.8 LF + 0.4 g ascorbic acid Study 6318 1 53 mg Mg + 4.0 ggmn + 1.5 g Stevia + 2.0 g 7 7 10 slight after-taste 11.3 LF + 0.4 g Naascorbate 2 50 mg Mg + 4.0 g gmn + 1.5 g Stevia + 3.0 g 5 5 10 off-taste 8.5 LF + 0.4 g Na ascorbate 3 54 mg Mg + 4.0 g gmn + 3.0 gStevia + 2.0 g 7 7 10 creamy, off -taste 8.5 LF + 0.4 g Na ascorbate 451 mg Mg + 4.0 g gmn + 3.0 g Stevia + 3.0 g 8 8 10 Best of Group 5.7LF + 0.4 g Na ascorbate 5 51 mg Mg + 4.0 g gmn + 4.0 g Stevia + 4.0 gxxxx xxxx xxxx off -taste 14.2 LF + 0.4 g Na ascorbate Study 6418** 1 31mg Mg*. + 4.0 g gmn + 0.4 g NaAscorbate + 10 7 10 sight off -taste 19.83.0 g stevia + 3.0 g LF 2 32 mg Mg*. + 4.0 g gmn + 0.4 g NaAscorbate +10 7 10 slight off-flavor 17.0 3.1 g stevia + 3.1 g LF 3 33 mg Mg*. +4.0 g gmn + 0.4 g NaAscorbate + 10 9 10 Best Taste 22.6 3.2 g stevia +3.2 g LF Abbreviations gmn—glucomannan LF—Lemon Flavor No LF—no lemonflavor perceived by the taste test Mg*—63 micron (230 Mesh) Lot ofmagnesium metal powder **0.72 mg FD&C Yellow # 5 is in the 100 mL DWadded for color.

1. Study 6218

Rows 1-12 of Study 6218 in Table 7, display twelve powder formulationswith variation, of Mg, stevia, lemon flavor (LF), Na ascorbate,isoascorbic acid, malic acid and ascorbic acid. After addition of 100 mLdistilled water and mixing, the solutions start to gel within 30-60seconds. Within an hour, an experienced dietitian evaluated theresulting gels, on a scale of 1 (bad) to 10 (excellent) for sweetness,tartness and texture.

All gels had an outstanding texture, being light and uniquely fluffy.However, none of the gels had an acceptable taste (Columns 3 and 4).There was an insufficient amount of sweetness. The gels shown in Rows2-12 expanded in volume by 5.6-25.5 mL after standing for at least anhour. The volume of the gel displayed in Row 1, with the lowestconcentration of Mg, contracted by 5.6 mL—probably due to an interactionof Mg with glucomannan. Otherwise, there is a dose-response relationshipfor increase in gel volume with increasing Mg content. (See Rows 1-4 ofStudy 6218). Addition of more Mg generates more H₂-thereby affecting gelexpansion and ‘fluffiness’. Although isoascorbic acid, ascorbic acid,and malic acid in the lemon - flavored formulation led to significantvolume expansion of the gels (Rows 7-10), they imparted a bitter, “off”taste at the concentrations tested.

2. Study 6318

Analysis of the results of Study 6218 led to the design and testing ofthe formulations listed under Study 6318 of Table 7. As a result ofStudy 6218, it was determined that Na ascorbate did not impart a bittertaste as found with testing the organic acids. An additional amount ofstevia was added to enhance sweetness. Also, an additional amount oflemon-flavored powder (LF) was added to enhance the lemon flavor.Magnesium metal powder was tested at 50-54 mg/100 mL.

It was found that none of the 5 gels listed in Rows 1-5 of Study 6318scored above an 8 for sweetness and tartness. The texture was excellent.The gel shown in Row 4 was judged to be best. All 5 gels increased ingel volume upon standing for one hour or more.

3. Study 6418

It was determined that based upon the results for Gel #4 of Study 6318that slightly more sweetness and lemon flavor were needed. A lower doseof Mg was used. This magnesium metal powder was the 63-micron (230 Mesh)fraction of the Lot of magnesium metal powder used in previous studies.It is designated in Table 7 as Mg*. Of the three gel formulas displayedin Rows 1-3 of Study 6418, #3 was judged qualitatively to be best. Thisgel had the highest level of both stevia and the lemon flavor. All threegels increased in volume upon standing.

The results demonstrate that it is possible to create a delicioustasting, textured, hydrogen-rich lemon gel based upon glucomannan andmagnesium metal powder. This hydrogen rich lemon gel should be helpfulto weight management and intermittent fasting regimens.

Lemon and chocolate hydrogen-rich gels have been prepared and have beenused to control food cravings in-between meals.

Example 9: Transforming Marketed Lemon-Flavored Powders, for Drinks,into Delicious Molecular Hydrogen-Generating and Sustaining Gels

1. Introduction

It has been found that magnesium metal powder (Mg)-glucomannan (gmn)formulations can be used to transform marketed drinks into gels with adesirable taste and texture. Of particular interest here, is turningmarketed low-calorie flavored powders designed to make beverages intolow calorie hydrogen-rich gels that can be used to augment weight lossand fasting programs. That is, drink making powders formulated with theaddition of Mg and gmn-transforms aqueous drinks into hydrogen-richgels, with an expanded volume, that are perceived as ‘filling’ andhaving a desirable and unique ‘fluffy’ texture.

TABLE 8 Molecular Hydrogen Gels Containing Marketed Lemon Flavored DrinkPowders 1-Hr 4-Hr Vol. Vol. Formula/100 mL Inc. Inc. # Distilled Water(DW) Taste Comments (mL) (mL) Study 6518 1 24 mg Mg* + 4.0 g gmn + 9Acceptable, 8.5 11.2 1.7 g Crystal Light Good 2 22 mg Mg* + 4.0 g gmn +10 Acceptable, 11.4 5.7 2.5 g Crystal Light better than 1 3 41 mg Mg* +4.0 g gmn + 9 Acceptable 14.2 17.0 1.7 g Crystal Light 4 40 mg Mg* + 4.0g gmn + 10 Best Gel, 11.3 14.2 2.5 g Crystal Light best flavor 5 20 mgMg* + 4.0 g gmn + 7 Not acceptable, 2.8 16.9 0.8 g Crystal Light weakflavor 6 42 mg Mg* + 4.0 g gmn + 8 OK, but weak 5.7 19.6 0.8 g CrystalLight flavor, color Study 6618 1 43 mg Mg* + 4.0 g gmn + 10 Excellent22.6 31.1 2.5 g Crystal Light (2012) Tartness 2 44 mg Mg* + 4.0 g gmn +10 Very Good 22.6 31.1 2.5 g Crystal Light (2020) Tartness 3 44 mg Mg* +4.0 g gmn + 10 Very Good 22.6 28.3 2.5 g Wyler's Light Tartness Lemonade4 42 mg Mg* + 4.0 g gmn + 9 Tartness not 20.0 31.1 2.5 g Great Value asgood Lemonade 5 4.0 g gmn + 2.5 g 10 Excellent 0.0 0.0 Crystal Light(2020) Tartness Study 61218 1 40 mg Mg* + 4 g gmn + 8 Needs more 11.411.4 2.5 g + True Lemon ® lemon taste Abbreviations Mg* 63 micron(230Mesh) Lot of magnesium metal powder gmn glucomannan Vol Volume Tasterated 1—awful; 10—Excellent

2. Experimental

The results presented in Table 8 outline the development and testing ofmolecular hydrogen (H₂)-rich lemon gels produced from marketedlemon-flavored drink powders. The gels were developed by addition ofglucomannan and Mg to the lemon-flavored powder. 100 mL of water wasthen added to the 4.8-6.6 g of powders and mixed for less than2-minutes—until a ‘fluffy’ gel formed. For these studies, 63-micron (230Mesh) magnesium metal powder (Mg*.) was used. Gels were evaluated fororganoleptic properties, i.e., sweetness, tartness and texture. Theseorganoleptic properties were grouped under ‘Taste’ in Column 3 of Table8. All gels containing Mg-gmn had unique desirable, light, ‘fluffy’texture. They were also evaluated for their potential to expand afterstanding for periods of one-hour and four-hours. Volume increasemeasurements were made as described previously.

3. Results

The results presented in Rows 1-6 of Table 8 of Study 6518 show theeffect of varying concentrations of Mg* and/or gmn on the taste andvolume change of various doses of Crystal Light® Natural Lemonade. Thegel formed from the ingredients displayed in Row #4, i.e., 40 mg Mg*+4.0g gmn+2.5 g Crystal Light® Natural Lemonade was judged to be the besttasting gel. It contained 3.1 times the recommended dose for makingCrystal Light® Natural Lemonade drinks. All formulations containingMg*-gmn, affected an expansion of gel volume—upon standing. Thisphenomenon indicated that the gels retained much of the H₂ that wasgenerated. Much of the H₂ was retained as gas bubbles. Mg* continued toreact with water, in the gel, and generated H₂ over the 5-hour timeframe studied (Compare Columns 5 & 6 of Table 8). This extendedreactivity of Mg* with water was indicative of glucomannan's ability toaffect the removal of the passivation coat of magnesium oxide from Mg*.As noted previously, the expansion of the gels provided for a highlydesirable ‘fluffy’ texture.

The results in Rows 1-5 of Table 8 of Study 6618 showed the effects ofaddition 42-44 mg Mg* and 4.0 g of gmn powders to the variouslemon-flavored marketed brands and mixing with 100 mL of distilled water(DW). The organoleptic properties and time course of volume expansion ofthe lemon gels was determined. Here, volume expansion was measuredrelative to that of the 4 g gmn+2.5 g Crystal Light® control gel (SeeRow #5, Study 6618). The organoleptic properties of all gels, except #4,met with approval by the dietitian. All gels containing 42-44 mg of Mg*showed marked expansion of the gels—relative to the control gel (in Row#5). Gels 1-4 showed expansion between 1- and 4-hours after preparation.The control gel (Row #5), without Mg*, did not expand after preparation.Thus, this study confirms the need for the generation of H₂ to expandthe gels.

Example 10: Time Course of Loss of Dissolved Molecular Hydrogen (H₂)from a Mg*-gmn Gel

The results presented in Table 9 show the time course of change indissolved H₂ when left to stand in an open container at 23 C.Measurements were taken with the H₂ Trustlex® meter. This Gel isgenerated from 40 mg Mg*+4.0 g gmn+2.5 g Crystal Light® powders mixedwith 100 mL of distilled water. A 5-hour time delay took place beforemeasurements were taken. The results show that at 5-hours post gelproduction (zero time of measurement), 709 ppb H₂ remains in the gel.Over the course of the next 535 minutes (about 9 hours), the H₂ drops to410 ppb, or retains 57.8% its H₂. Thus, in an open container, Mg-gmngels retain dissolved H₂ for extended periods of time. These resultssupport the presence of a strong interaction of the Mg*-gmn containinggel with H₂.

TABLE 9 Time Course of Loss of Dissolved Molecular Hydrogen (H₂) from aMagnesium Metal Powder (Mg*) - Glucomannan Gel in an ‘Open Cup’ Study**% H₂ Minutes ppb H₂ Remaining 0 709 xxxx 10 712 100.0 15 690 97.3 25 59984.5 85 454 64.0 160 455 64.2 195 444 62.6 300 435 61.4 360 436 61.5 420431 60.7 535 410 57.8 Abbreviations Mg* 63 micron(230 Mesh) Lot ofmagnesium metal powder ppb parts per billion molecular hydrogen**Started 5-Hours after Gel formation. gmn glucomannan

Example 11: Production and Analysis of Molecular Hydrogen (H₂) Rich Gelsof Different Flavors

1. Introduction

This Example illustrates the utility and flexibility of the embodimentsdescribed herein: The magnesium metal powder (Mg)-glucomannan (gmn)formulations are effective at transforming powders designed to producebeverages into low or no calorie hydrogen-rich, expansive gels that canbe used for diet deserts and snacks.

2. Experimental

Each of 10 different Crystal Light® flavors, 2.5 g/serving, wereindividually mixed with 40 mg Mg* and 4.0 g of glucomannan to create 10different powder formulations. To initiate gel formation, 100 mL ofdistilled water was added to an 8 oz. plastic cup containing eachformulation and mixed for 60-90 seconds to complete gel formation. Afterone hour, the gel height was measured and the gel volume calculated, asdescribed above. The gel volume increase, above the control without Mg*,was determined by subtracting the control gel volume from theexperimental gel volume. The gels were evaluated for sweetness, texture,tartness, and acceptance by an experienced dietitian.

3. Results

In Column 3 of Table 10 are shown the volume increases due to incubationof the test gels for one-hour. Gel expansion was measured - relative toa control gel containing 4.0 g of gmn+2.5 g of Crystal Light® in 100 mLof distilled water. All test gel volumes increased by 14.2-25.5%. i.e.,by 14.2-25.5 mL. These values reflect molecular hydrogen (H₂) beingentrapped in the gel as both dissolved molecular hydrogen and H₂bubbles. The variability of the increase in volumes for the differentgels is due to differences in pH and the concentrations of components ofthe assorted flavors.

TABLE 10 Preparation of Hydrogen-Rich Gels using Magnesium Metal Powder(Mg*) Plus Glucomannan (gmn) Plus Crystal Light ® Flavors - added to 100mL Distilled Water (DW) Formulas Containing 40 mg Mg* + 4.0 g gmn Gel **# Mixed with 100 mL of Distilled Water Inc. (mL) Sweet Texture TartnessAccept 1 2.5 g CL - Peach Mango Green Tea 17.0 OK Good NI YES Comment:Good 2 2.5 g CL - Lemonade 19.8 OK NI 0K YES Comment: Good 3 2.5 g CL -Peach Iced Tea (Black Tea) 17.0 OK NI 0K YES Comment: Good 4 2.5 g CL -Grape with Caffeine 25.5 OK NI NI YES Comment: Good 5 2.5 g CL - WildStrawberry with Caffeine 25.5 OK NI 0K YES Comment: Good 6 2.5 g CL -Classic Orange 22.6 NS NI 0K YES Comment: Good 7 2.5 g CL - Fruit Punch14.2 OK NI NI NO Comment: Too dense 8 4 g gmn + 2.5 g CL - Pink Lemonade19.8 OK OK OK YES Comment: Good 9 2.5 g CL - Lemon Iced Tea 19.8 TS NINI NO Comment: Off Color 10 2.5 g CL - Raspberry Lemonade 25.5 NS NI NINO Comment: Too dense Abbreviations CL Crystal Light ® Mg*—230 Mesh Lotof magnesium metal powder. gmn glucomannan ** Gel volume increase -relative to the control 4.0 g gmn + 2.5 g CL/100 mL DW Gel EvaluationsTS Too Sweet, reduce the sweetener NS Needs sweetness - add OK Excellentsweetness or tartness NI Needs improvement in sweetness or tartness

Reviewing the results in Columns 4-7, it is observed that eight of tenof the gels were judged to be acceptable—meaning they were delicious andhad the desired ‘fluffy’ texture. Means of improving the organolepticproperties of those gels that were ‘not acceptable’ was readilyidentified and delineated in Column 4-7 of Table 10.

4. Discussion

These results attest to the flexibility of the embodiments describedherein in creating good tasting gel products that are healthful to theconsumer for both weight control as well as preventing and treatingobesity associated-inflammation.

Essentially, any food or drink product that contains water, or isintended to contain water, can be formulated with the magnesium metalpowder-glucomannan biotechnology—to generate and release molecularhydrogen and expand the gel volume.

Additional ingredients can be added either before or after forming themagnesium metal powder-glucomannan gels. Health-promoting ingredientsare of most—but not exclusive interest.

Example 12: Chocolate Smoothie

A chocolate smoothie ‘control’ was prepared with the followingingredients:

300 mL of Great Value® (Walmart) fat-free milk;

5.1 grams of Hershey® Coca Natural Unsweetened;

3.0 grams of Sweet Leaf® stevia with inulin, a prebiotic;

Calorie content—about 100 calories.

Preparation, at 15 C, took place in a 600 mL Magic Bullet® container byadding the ingredients to the 600 mL container and mixing at high speedfor 30 seconds. Then, the mixture was allowed to settle for 5 minutes.It was observed that a non-bubbly liquid-bubbly liquid phase separationtakes place at 5 minutes. Therefore, the solution was mixed each timebefore viscosity measurements took place.

Viscosity measurements were made using an Elcometer® Shell 6 231005047viscosity cup. The measurement consists of the time needed for thesolution to completely flow through the cup. Increased viscosity resultsin a slower flow rate. The time needed for the above solution to passthrough the viscosity cup was 24.1 seconds (N=5).

After viscosity measurements were taken, the above formulation wasmodified by addition of:

3.0 grams of glucomannan;

0.11 grams of crude magnesium metal powder;

1.0 gram of sodium ascorbate; and

1.1 gram of potassium citrate.

Preparation, at 20 C, took place in a 600 mL Magic Bullet® container byadding the ingredients to the 600 mL container and mixing at high speedfor 30 seconds. Then, the mixture was allowed to settle for 5 minutes.It was observed that no phase separation took place. However, thesolution was mixed each time before viscosity measurements took place.

Viscosity measurements took place over a 30-minute time frame. Theaverage time for the formulation to clear the viscosity cup was 49.2seconds (N=10). Thus, addition of the Mg-gmn formulation more thandoubled the viscosity of the original formulation. During the viscositymeasurements, it was observed that the time for the formulation to passthrough the cup increased after each viscosity measurement indicatingthat the viscosity increased with time. Therefore, the modifiedformulation should be allowed to settle for 30 minutes, or more, beforeconsumption.

Approximately one hour after preparation, the hydrogen content and pH ofthe modified formulation was measured. The molecular hydrogenmeasurement with the Trustlex® H₂ Meter demonstrated that 168 ppb H₂ wasstill present in the formulation at a pH of 7.10. Expert taste testersagreed that the modified formulation tasted very good and has a nicetexture.

The formulation was frozen in a freezer overnight. After microwaving theformulation for 70 seconds, it was consumed. The taste and texture wereconsidered acceptable.

For practical purposes, the Mg-gmn hydrogen formulations can be added tothe food ingredients and mixed. The mixture can be consumed immediately.Hydrogen will be generated for an extended period in the ‘gut’ from theMg in the mixture.

It should be noted that the Mg-gmn formulations will generate H₂ inseveral types of drinks. These drinks include soft drinks, fruit juices,milk and milk substitutes, smoothies, alcoholic beverages, soups andseveral types of water.

Example 13: Blueberry Protein Breakfast Smoothie

A sweetened blueberry and whey protein breakfast ‘control’ smoothie wasprepared with the following ingredients:

300 mL reverse osmosis water;

3 grams of stevia (PJURE®);

42.5 grams of frozen blueberries (Great Value® Whole Blueberries);

21 grams of EAS® 100% Whey Protein.

About 100 calories.

Preparation, at 23 C, took place in a 600 mL Magic Bullet® container byadding the ingredients to the 600 mL container and mixing at high speedfor 30 seconds. Then, the mixture was allowed to settle for 5 minutes.The volume was transferred to a 600 mL graduated beaker and estimated tobe 525 mL. Then, 100 mL of the formulation was removed, and 425 mL ofthe formulation was returned to the 600 mL Magic Bullet® for additionalmixing with Mg-gmn.

Two grams of a formulation containing 4.65% magnesium metal powder,2.33% glucomannan, 2.33% maltodextrin, 23.3% isoascorbic acid and 46.5%potassium citrate was added to the 600 mL Magic bullet container holdingthe 425 mL of formulation. Mixing took place for 30 seconds, followed bya 5-minute period of settling and allowing Mg to react with water in theMagic Bullet® container. The volume was then transferred to a 600 mLgraduated beaker and measured to be 525 mL. Thus, there was a 100 mL, or23.5% gain in volume after addition of 2 grams of the formulationcontaining Mg, gmn and excipients. A large quantity of gas bubbles wasseen to be dispersed throughout the thixotropic formulation. Thus, asmuch as 98 mL molecular hydrogen (H₂) is present in the bubbly phase ofthe gel.

To test for release of H₂ from the bubble phase of the formulationand/or for latent generation of H₂ in the gel, the presence of availableH₂ in the formulation was tested using the Trustlex® H₂ Meter. 50 mL ofthe final formulation was placed in an 80 mL plastic cup. Measurementsof H₂ were periodically taken while immersing the H₂ meter in theformulation (23 C) for approximately 5 hours. The results are asfollows: from 0 to 10 minutes, there was zero H₂ detected by the Meter;after 20 minutes, H₂ rose to 21 ppb; after one hour, H₂ level increasedto 234 ppb; at 2.5 hours H₂ level was 441 ppb; by 3 hours H₂ level was920 ppb; at about 4.25 hours H₂ level was 1031 ppb; and by 5 hours H₂level had decreased to 1017 ppb.

Thus, this breakfast smoothie containing magnesium metal powder,glucomannan, and catalytic excipients provides an extended generationand release of molecular hydrogen. When ingested, the consumer will beprovided with a continued release of H₂, in the gastrointestinal tract,for five or more hours.

Example 14: Lemon Flavored Vegetarian Protein Powdered Drink

A lemon flavored organic vegetarian citrus ‘control’ drink was preparedwith the following ingredients:

300 mL of reverse osmosis water;

10.0 grams Nutra® protein powder blend Greens;

1.5 grams of BioFest® Lemon Powder Calorie content is about 20 calories.

Preparation, at 15 C, took place in a 600 mL Magic Bullet® container byadding the ingredients to the 600 mL container and mixing at high speedfor 30 seconds. Then, the mixture was allowed to settle for 5 minutes.The formulation was mixed each time before viscosity measurements tookplace.

Viscosity measurements were made using an Elcometer® Shell 6 231005047viscosity cup. The measurement consists of recording the time needed forthe solution to completely flow through the cup. The average time neededfor the above solution to pass through the viscosity cup was 4.0 seconds(N=5).

After viscosity measurements were taken, the above formulation wasmodified by addition of:

2.0 grams of glucomannan;

0.204 grams of magnesium metal powder;

4.1 grams of citric acid; and

4.5 grams of maltodextrin.

Preparation, at 20 C, took place in a 600 mL Magic Bullet® container byadding the ingredients to the 600 mL container and mixing at high speedfor 30 seconds. Then, the mixture was allowed to settle for 5 minutes.It was observed that no phase separation took place. However, thesolution was mixed each time before viscosity measurements took place.

Viscosity measurements took place over a 30 minute period. The averagetime for the formulation to clear the viscosity cup was 18.3 seconds(N=5). Thus, addition of the Mg-gmn formulation increased the viscosityof the original formulation by more than a factor of four. However, thismodification resulted in a flowable liquid and not a gel. Taste testingindicated that this vegetarian formulation had a strong but pleasanttexture and citrus taste.

Example 15: H₂-Rich, Thickened Tomato Soup

Soup is an appropriate vehicle for delivering H₂ systemically. For soupswith a pH below 7, there is no need to add an H₂-generating acid orantioxidant. Otherwise, some combination of isoascorbic acid and sodiumor potassium citrate could be added to facilitate the reaction of Mgwith water.

Briefly, 100 mL of commercially available tomato soup was microwaved toprovide a temperature of 92 C for the soup. Then, 52 mg of Mg*(63-micron particle size) was added to the soup and stirred for 15seconds. Next, 1 g of glucomannan was added and stirred for 60seconds—thickening the soup into a rich texture. The soup mixture wasallowed to cool to 55 C. The Trustlex® H₂ Meter indicated that the soupcontained 907 ppm H₂. The pH was 4.38. The soup was then consumed andfound to be palatably acceptable.

Example 16: Scale-up for Production and Manufacturing

1. Introduction

All of the above examples have described the preparation and testing ofunit doses of powdered formulations containing magnesium metal powderand glucomannan plus other beneficial ingredients that add flavor,sweetness and other desirable attributes. For ‘in use’ testing by alarge number of consumers, as well as for commercial manufacturing, itis necessary to prepare much larger batches that can be packaged in unitdose packets or in large, e.g., 100-10,000 g containers - where unitdoses can be dispensed, for example, with scoops.

2. Experimental

An excellent tasting low-calorie lemon flavored powder, proven to geland sustain molecular hydrogen, when mixed with water, was developed.Thus, it was ready for an ‘in use’ test. A batch containing 90-unitdoses was determined to be needed. The weight of a unit dose was foundto be 5.835 grams. A 3% w/w overage was built into the batch. Konjacglucomannan was from Best Naturals®; malic acid, maltodextrin, aspartamewere from Bulk Supplements; anhydrous magnesium sulfate was fromSigma-Aldrich; 230 Mesh magnesium metal powder (Mg*) was prepared from abatch of crude magnesium metal powder (from China); mixed tocopherols,45%, were from Profood Products Outlet; FD & C Yellow #5 Dye was fromFlavors and Colors.com. A 2L VH-2 dry powder blending, and mixingmachine was obtained from RumeiShopping (China). The ingredients of theformulation were placed in the VH-2 mixer and mixed at a setting of 250(i.e., 15 rotations per minute) for 30-minutes before being packaged ina sterile plastic container.

3. Results

The formula, containing the grams of each ingredient that was preparedand each ingredient's functionality are shown in Table 11.

TABLE 11 Scale - up of a Powder Mixture for Making a Molecular HydrogenGenerating and Sustaining Gel Ingredient Grams Function Konjacglucomannan 278.430 gelling, H₂ sequestration malic acid 136.103Flavoring agent, acidifier maltodextrin 92.716 sweetener, bulking agentmagnesium sulfate - anhydrous 9.234 desiccant, anti-caking aspartame7.729 sweetener 230 Mesh Magnesium Metal Powder 5.529 Generate H₂ Powderacesulfame 3.759 sweetener mixed tocopherols 4.599 anti-oxidant,freshener FD&C Yellow # 5 0.464 Coloring agent Total 538.563

A unit dose, i.e., 5.835 grams, of the batch, was delivered to an empty8-ounce plastic cup. Thereafter, 100 mL of distilled water was added andmixed with a spoon. Within 120 seconds, a gel formed and expanded by 25%within an hour, demonstrating the generation and sequestration ofmolecular hydrogen. The gel was judged to have excellent organolepticproperties—including taste, tartness, and texture. Thereafter, it wasentered into an ‘in use’ test.

4. Discussion

The results demonstrate the feasibility of scaling up formulationscontaining magnesium metal powder and glucomannan for generating andsustaining molecular hydrogen.

Example 17: Oral Health: Treatment Gingivitis with a H₂-Chlorhexidine ina Magnesium metal powder-Glucomannan Gel

It is well known that gingivitis (i.e., gum inflammation) leads toperiodontal disease. It is the leading cause of tooth loss in bothhumans and animals. Older dogs and cats are particularly susceptible toperiodontal disease.

Drugs, such as chlorhexidine, an anti-microbial, and anti-inflammatories(NSAIDS) have been used in the oral cavity to reduce inflammationaffecting gingivitis and resultant periodontal disease. These treatmentshave been only partially effective. There is a need for both bettersustained delivery systems of antimicrobials and for more effective,longer lasting anti-inflammatory therapies. Studies attest to theantibacterial activity of molecular hydrogen water against oralbacteria.

A gel containing 0.12% chlorhexidine gluconate and 22.1% molecularhydrogen(H₂), a potent anti-inflammatory and antioxidant, was prepared:Three mL of Hibiclens® (4% w/v chlorhexidine) was diluted to 0.12% with97 mL of distilled water. The solution was then added to an 8 oz.plastic cup containing 99 mg of crude magnesium metal powder and 4.0 gof glucomannan powder. Mixing took place for about 30 seconds, at whichtime a gel started to form. A line was placed at the top of the gel todelineate its height in the cup at that time. The gel was allowed toexpand overnight. Thereafter, a second line was placed on the top of thegel where there was a new gel height. The volume of H₂ in the gel wascalculated by multiplying the difference, in centimeters, between thetwo lines times the area of the base of the cup (i.e., 28.3 square cm.).The volume of hydrogen was calculated to be 28.3 mL. Thus, the totalvolume of the gel, after expansion is 128.3 mL, resulting in aconcentration of H₂ of 22.1% in the gel.

An N=1, Phase 1 therapeutic trial was carried out. The subjectperiodically develops gingivitis and has a history of periodontaldisease despite good oral hygiene. Thirty-five mL of the gel was placedin the oral cavity with a spoon and then spread over the surface of thegums and teeth with the subject's tongue. The subject found the tastemuch more acceptable compared to other therapies, for example, atherapeutic oral rinse. The gel was retained in the oral cavity for tenminutes. Symptoms associated with gingivitis, such as sensitive gums,was ameliorated within twelve hours.

The gel can be applied to the gums by other means such as use of atongue depressor, a regular toothbrush, an electric toothbrush or anyother appropriate means. If the gums are sensitive, application with a‘Q’ Tip may be preferred. Regardless, the gel should be retained in theoral cavity for as long as possible. Chlorhexidine and H₂ will diffusebetween the teeth. Ten minutes is recommended. Then, it can be washedout with water or mouthwash. Hydrogen peroxide should not be used sinceit reacts with H₂ and deactivates it.

It was determined that this product is of utility for veterinary oralcare for older animals (e.g., dogs and cats) since it is substantive tothe oral cavity. Dogs and cats are subject to tooth loss due gingivitisresulting in periodontal disease. The gel can be administered to animalsin an analogous manner as done for humans. An alternative method ofdelivery consists of incorporating a ‘treat’ into the gel. For example,a gel was prepared as described above, with the addition of 2% peanutpowder. The gel was readily taken into the oral cavity where asignificant amount stuck to the gums and teeth, thereby deliveringchlorhexidine and H₂ to the gums for an extended period.

Compositions as described herein could alternatively be formulated in toa toothpaste for delivery to the oral cavity and gums.

Example 18: Gastrointestinal Diseases: Sustained Release of H₂ andBismuth Subsalicylate from a Magnesium Metal Powder-Glucomannan Gel

There are diseases and conditions of the upper gastrointestinal tractwhere sustained delivery of both effective drugs and H₂ would have anadvantage over current treatments. Compositions described herein provideeffective treatment of conditions such as gastritis; gastric andduodenal ulcers, gastroesophageal reflux disease (GERD), Helicobacterpylori infection, bacterial overgrowth, yeast overgrowth, heartburn,indigestion, upset stomach and nausea. Non-limiting examples of drugsthat could be delivered from hydrogen-rich Mg-gmn gels are proton pumpinhibitors, misoprostol, H₂ receptor antagonists, antibiotics,antifungals, anti-inflammatories, antacids, bismuth subsalicylate, orany combination thereof. These drugs alone or in some combinations, attherapeutic doses, can be incorporated into aqueous Mg-gmn gels.

As an example, 50 mg Mg* plus 4 g of glucomannan were mixed and added toa solution containing 30 mL of a solution containing 1.050 g bismuthsubsalicylate and 70 mL of distilled water. The mixture was stirred for60 seconds, at which point the resultant solution gelled. A line wasdrawn to mark the gel height. The initial height was 5.3 cm indicating agel volume of 179.4 mL. The weight of the gel was 107.89 g implying adensity of 0.602 g/mL. Comparably speaking, this is a low density-relative to previously tested 4% gmn-—20 mg Mg* gels (See Table 2). Thegel was allowed set for 3 hours. The height of the gel was determined tobe 5.6 cm. with a gel volume of 185.8 mL and a density of 0.581 g/mL.The H₂ content of the gel, as measured with the Trustlex H₂ Meter was1405 ppb at a pH of 7.25. The low density of this gel, at outset, andits high H₂ content, demonstrates that copious amounts of H₂ wasgenerated at the outset of mixing and gelling of the gel. (NB: Lettingthe gel set for more than a few minutes is not necessary since the gelwill continue to generate H₂ in the stomach for a prolonged period).

Subsequent oral administration of the mixture described above to asubject experiencing acute heartburn resulted in resolution of symptomswith no discernible side effects.

Example 19: Mg-glucomannan to treat of Helicobacter pylori infection

Bismuth subsalicylate, in combination with antibiotics (250 mg ofmetronidazole and 500 mg of tetracycline) has been used to eradicateHelicobacter pylori infections. 250 mg metronidazole, 500 mgtetracycline, and 1.055 g bismuth subsalicylate are incorporated into aMg*-gmn formulation. Such a formulation could be marketed as tablets,capsules or a powder. A gel could be formed in a glass of water—byadding the formulation and mixing and then ingesting the gel.Alternatively, the patient could ingest a capsule (or tablet) containingthe formulation followed by an 8 to 16-ounce glass of water. The gelwill spontaneously and rapidly form in the stomach and it will ‘float’affecting a long retention time in the stomach. Long lasting, i.e., 5 to10-hour delivery of H₂ and the drugs should be achieved.

An example formula for treatment if Helicobacter pylori and bacterialovergrowth provided in a dosage of six ‘000’ capsules is:

1.0 g bismuth subsalicylate

250 mg of metronidazole

500 mg of tetracycline

3.0 g glucomannan

50 mg of 63-micron magnesium metal powder

Alternatively, the above formula can be mixed with water in a 12-ounceglass that will spontaneously form a gel, within 5-minutes—that can beingested without side effects.

Example 20: Treatment of Skin Disorders with MolecularHydrogen-Salicylic Acid in a Magnesium Metal Powder-Glucomannan Gel

Until now, there was no practical manner for sustained topical deliveryof H₂ to the integument.

An anti-acne, keratolytic preparation consisting of 54 mg Mg* (63-micronparticle size), 2 g salicylic acid, 2 g konjac root glucomannan in 100mL distilled water was prepared in a plastic cup by mixing thecomponents for 45 seconds while a gel formed. The gel was allowed to setovernight. The volume expansion of the gel was found to be 34.0 mL or34%. Therefore, the expanded gel contains 34 mL of H₂. The pH of the gelwas found to be 3.34.

Two ‘quarter’-sized areas (4.15 square cm.) were delineated on the hairclipped skin of the right forearm of a male subject. One site served asan untreated control while the other site was treated topically with0.24 g/square cm. of the gel. The gel was spread over the site with atongue depressor in a continuous layer. The H₂ in the gel, on the skinsurface, was determined with the Trustlex® H₂ Meter—without theProtective Guard. Removing the Protective Guard allowed for directcontact of the Trustlex® electrode with the skin surface. Thus, theconcentration of H₂ being delivered to the skin surface can bedetermined. The presence of salicylic acid on the skin surface and inthe stratum corneum was observed with a Wood's Light (UVA). Salicylicacid fluoresces in the UVA, allowing it to be seen on the skin surfaceunder UV light. Tape stripping (3M Scotch Tape) the skin on the siteallows for determining the layers of stratum corneum penetrated bysalicylic acid. That is, each tape strip of the salicylic acid-treatedsite represents a layer of stratum corneum penetrated by salicylic acid.

It was found that, after washing off the remaining gel from the skinsite, it took ten tape strippings of the treated site to remove thevisible presence of the UVA fluorescence. Thus, the gel deliveredsalicylic acid through 9-10 layers of stratum corneum, close to thelowest layers of the stratum corneum of forearm skin.

The time course of change in H₂ on the skin surface after application ofthe H₂-rich gel, was followed. At baseline, it was determined that 432ppb H₂ was in contact with the skin surface. Within 10 minutes 250 ppbH₂ was detected at the skin surface. At 20 minutes 167 ppb H₂ wasdetected at the skin surface. At 30 minutes, it had dropped to zero. Itis assumed that a substantial portion of the H₂ in contact with the skinsurface was absorbed into the skin. Also, once water has evaporated fromthe skin surface, it is no longer available to react with Mg to generateH₂. The stratum corneum, the top barrier of the skin, is hydrophobic. H₂is also hydrophobic. Thermodynamically, hydrophobic entities associatewith each other, in an aqueous environment. This shows the compositionas described above can deliver both H₂ and salicylic acid to theintegument. Mg-gmn gels containing numerous drugs, alone or incombination are feasible for treating various skin afflictions.

Non-limiting examples of skin diseases and conditions that can betreated and drugs that can be incorporated into H₂ Generating Mg-gmnskin care products are:

aging skin: alpha-hydroxy acids, antioxidants, ascorbic acid,trans-retinoic acid;

acne: doxycycline, lymecycline, minocycline, erythromycin, trimethoprim,cotrimoxazole, salicylic acid, trans-retinoic acid;

dry, flaky or thickened skin: alpha-hydroxy acids, salicylic acid,glycerin;

allergic contact dermatitis: corticosteroids, topical antihistamines;

atopic dermatitis: corticosteroids, antihistamines;

psoriasis: salicylic acid, corticosteroids, coal tar,immunosuppressants;

sunburn: topical anesthetics, aloe vera, NSAIDS;

bruising: arnica, vitamin E, vitamin C;

irritated skin: glycerin, cholesterol sulfate;

fungal infections: clotrimazole, econazole, miconazole, terbinafine,fluconazole, ketoconazole, amphotericin;

corns and callouses high dose salicylic acid;

combinations of the drugs listed above for complex diseases; or

dermatology preparations, containing abundant H₂ need specialpreparation and/or packaging.

In some embodiments, solids containing Mg and glucomannan must be in aseparate compartment from water. They would be mixed ‘in situ’ inunit-dose packages. The lotion or gel generated would contain abundantH₂ for about a week. A preservative, such as sodium adipate, may beadded.

An alternative means of stabilization for marketing would be to generateH₂ within the formulation, by mixing liquid and solid phases duringmanufacturing and sterilizing. This product would then be packaged in asealed aluminum container that can give it a shelf life of over a year.It is best packaged in small doses that would last the consumer about aweek.

Example 22: H₂ Moisturizing Gel for Dry, Aging skin

As skin ages normally or from environmental damage, it is subject tosub-chronic inflammation and hyperproliferation which affects difficultyin holding moisture. A moisturizing product that will reduce sub chronicinflammation without drugs that cause irritating side effects, isneeded.

The following H₂-generating moisturizing skin lotion was prepared:

3.0 g lactic acid;

1.5 g glucomannan;

51 mg Mg* (63 micron);

20 mL glycerin

80 mL distilled water

For preparation, glycerin and distilled water were mixed and added tothe remaining ingredients in an 8 oz. container and mixed for 60 secondsuntil the contents were dissolved. A lotion resulted. The lotion wasallowed to stand at 23 C for one hour. The Trustlex H₂ Meter indicatedthat the lotion contained 815 ppb H₂ at a pH of 3.86.

Two quarter-sized areas (4.15 square cm.) were delineated on the hairclipped skin of the right forearm of a subject. One site served as anuntreated control site while the other site was treated topically with0.15 g/square cm. of the lotion. The lotion was spread over the site,with a tongue depressor, as a generous layer of lotion. H₂ on the skinsurface, was determined with the Trustlex® H₂ Meter without theProtective Guard. Removing the Protective Guard allowed for directcontact of the Trustlex® electrode with the skin. The electrode waswetted with distilled water before touching the skin surface.

The time course of change in H₂ on the skin surface is shown in Table12. At baseline, the H₂ on the skin surface was 804 ppb, close to thatin the lotion (i.e., 814 ppb). As time progressed, the H₂ on the surfaceof the skin fluctuated and did not show a progressive loss, as expected,up to 60 minutes. Thereafter, H₂ measurements on the skin surface showedthe presence of significant H₂ up to 210 minutes.

TABLE 12 Time Course of Change in H₂ on Skin Surface after Applicationof a H₂-Rich Anti-aging Moisturizing Lotion Treated* Untreated Time H₂H₂ (Min. ppb ppb 0 804 0 5 756 0 10 917 0 15 327 0 20 351 0 30 330 0 60791 0 120 169 0 210 247 0 360 0 0 *Treated with 51 mg Mg*(63 microns),3.0 g lactic acid, 1.5 g glucomannan, 20 g glycerin and 80 g distilledwater, H₂ = 815 ppb, pH = 3.86. Skin Surface pH = 4.57.

This level of persistence of H₂ on the skin surface was surprising andunexpected. The lotion rapidly loses most of its water as it dries onthe skin surface. Bubbles disappear. Only a thin layer of productremains on the skin surface. However, such persistence may be explainedby:

Mg*, deposited on the skin surface by the lotion, continues to reactwith water held on the skin surface by the hydroscopic effect ofglycerin and lactic acid;

As noted in previous Examples, H₂ has an affinity for glucomannan.Therefore, glucomannan may contribute to H₂ persistence on skin;

The stratum corneum has a reservoir effect for hydrophobic molecules. H₂is hydrophobic. It may contribute to the H₂ detected on the skin surfacedue to back diffusion of H₂ from the stratum corneum.

Example 23: Sustained Delivery of H₂ to a Model Aquarium or Fish Farm

It has previously been demonstrated that molecular hydrogen (H₂) canpromote the health and growth of both animal and plant life (1, 14).Aquatic life in the form of plants, invertebrates (e.g., shrimp, crabs,etc.) and fish should also benefit from the antioxidant and enhancedbioavailability effects of H₂ in an aqueous environment. Plants, fish,insects and all invertebrates, like higher animals, have mitochondria.H₂ is known to reduce the toxic reactive oxygen species (ROS), i.e.,hydroxyl radical and peroxynitrite produced by mitochondria. Thesepromoters of inflammation affect the consumption of energy that couldotherwise be used for growth and fighting disease.

An experiment was designed to determine if a magnesium metal powder(Mg)-glucomannan(gmn) gel that generates H₂ can deliver and sustain H₂in a model aquarium or aquatic farm. For the model aquarium or fishfarm, 9.95 grams of Fisher® phosphate buffered saline (PBS) in 1,000 mLof distilled water was prepared. The pH was 7.6.

For preparing the gel, 0.1 g of crude magnesium metal powder (Mg), 0.5 gof ascorbic acid and 4 g of glucomannan were mixed into 100 mL ofdistilled water (DW)—until the gel started to form. The H₂ concentrationin the gel was determined to be 1501 ppb—using the Trustlex® H₂ Meter,at a pH of 8.4. The gel expanded in height by 0.9 cm. Thus, the volumeof H₂ in the gel is 25.5 mL or 25.5% of the original 100 mL volume.

After the baseline reading, the 125 mL gel was placed in the 1,000 mLPBS solution representing the aquarium or fish farm. Being less densethan water, the gel floated on top of the 1,000 mL beaker. The PBS wasconstantly circulated, at 23 C, by stirring with a 1 in. magneticstirring bar at the lowest power setting on the magnetic stirrer.

The results are shown in Table 13. At baseline, there was found to be 0ppb H₂ in the PBS solution, at a pH of 7.6. After 15 minutes, the H₂ inthe PBS remained at 0 ppb, at a pH of 7.6. By 4.7 hours, there was 562ppb H₂ in the PBS, at a pH of 7.7. At 13.8 hours, H₂ in the PBS hadrisen to 691 ppb, at a pH of 7.7. As time progressed, there was anaccumulation of small white debris in the PBS. This accumulationappeared to be a product of shedding gmn particles from the floatinggel. Upon cessation of stirring, this material tended to float to thetop of the beaker—near the gel supporting the notion that it is gmnparticles. At 28.3 hours, the H₂ in the PBS had risen to 1245 ppb at pH7.6. Thereafter, the H₂ in the PBS was sustained at a level of 1202 ppb,pH 7.3 until 109 hours. At 123 hours there was 1165 ppb H₂, pH 6.8. ThepH drop probably indicates bacterial growth in the simulated tank.

TABLE 13 Test System for Delivery of Molecular Hydrogen (H₂) to AquaticLife Time ppb H₂ pH (Hrs.). in PBS Units 0 0 7.6 0.25 0 7.6 4.7 562 7.713.8 691 7.7 28.3 1245 7.6 86.0 1234 7.3 109.0 1202 7.3 123.0 1165 6.8

This experiment demonstrates the feasibility of delivering H₂ to anaquarium or aquatic farm. It also points to routine steps that must betaken to insure the maintenance of water quality in an aquarium or fishtank. These maintenance steps include those that would normally becarried out without addition of the gel: filtration of excess particlesout of the tank, include antibacterial and anti-algae agents that arecompatible with the aquatic life in the tank. If proper maintenance iscarried out, the water should be acceptable for 2-4 weeks.

For situations when the body of water contained in the tank is largerthan 20:1 tank to gel ratio, fish or invertebrate meal can beincorporated into the gel. This maneuver should attract fish orinvertebrates to the gel where they will consume a higher level of H₂.

The applications foreseen for this method of delivery of H₂ to aqueoussystems, of such, include:

home aquariums containing aquatic plants, fish, turtles, invertebrates;

crustacean and mollusk, oyster farms;

fish farms including catfish, tilapia, salmon and carp; or

farming aquatic plants including rice, algaculture seaweed andornamental plant farming.

Of importance, is the potential of H₂ delivery to aquatic systems toincrease the yield of aquatic food to feed the world's growingpopulation and to protect the environment against over-fishing anddestruction of aquatic plant life.

Example 24: Molecular Hydrogen-Rich Magnesium Metal Powder-GlucomannanGels for Increasing Insect Yields

As the world's population increases beyond 7,650,000,000, it becomesincreasingly difficult to provide complete nutritional food,particularly in the form of complete protein and associated amino acids.There is increasing interest in farming insect populations to feed thegrowing masses. Insects are an excellent source of complete protein,vitamin B12, vitamin A and riboflavin. They reproduce and grow rapidlyand eat almost anything. They are particularly attracted to necroticlife forms, rotting food and feces. Thus, they are ‘natural’ cleaners ofthe environment. Crickets, cockroaches, grasshoppers, beetles, moths,etc. are now being farmed for both human and animal consumption.

Insect food can also serve as food for lower animals, including poultryand fish farming.

Farming of insects has several advantages over the farming animals, suchas cattle and chickens, including reduced feed per yield of protein,greater nutritional efficiency, less concern about epidemics in aninsect population compared to an animal population, lower greenhouse gasemissions and lower land usage.

Although insects breed and grow rapidly, a technology that wouldincrease protein and nutritional yield would be of economic benefit toboth insect farmers and nutritionally deficient populations. Sincemolecular hydrogen has been shown to increase reproduction and growth inmany life forms (1, 14), mainly through its antioxidant effects therebyreducing mitochondrial reactive oxygen species, there is no good reasonto doubt its growth promoting effects in insect populations. Insectcells are powered by mitochondria.

A prototype insect farming system was modeled to determine if wildtypeinsects would be attracted to a molecular hydrogen (H₂) gel that wasprepared in an 8 oz. plastic cup. The gel was formulated as follows: 51mg of Mg plus 4 g of glucomannan and 5 g of fructose were mixed in an 8oz. plastic cup. Next, 100 mL of white vinegar (5% acetic acid) wasadded to the cup and the contents mixed with a tongue depressor untilthe gel formed. The height of the gel was delineated with a blue linedrawn with a marking pen. The gel was allowed to stand for one hour forthe gel to form and evolve H₂. The new gel height was again delineatedwith a marking pen. The H₂ content of the gel was then measured byimmersing the unguarded Trustlex® electrode into the gel. The H₂ contentof the gel was found to be 800 ppb at a pH of 3.35. The plastic cupcontaining the gel was placed outside of the laboratory in a garden likeatmosphere. The temperature ranged from 90-105 F. Over the course of24-hours, the gel was observed for the presence of insects. Bees, flies,fruit flies, ants and other un-identified insects appeared to beattracted to the gel.

The purpose of placing insect food, in this example, fructose and aceticacid, in the H₂-rich gmn gel, is to attract insects to the gel therebyexposing the insects to a high dose level of H₂. As the insects ingestboth the insect food and the glucomannan, they will come into closecontact with H₂ which will be both ingested and absorbed into their bodyparts that are in contact with the gel.

The example gel illustrated here, is not optimized for the mostefficient delivery of H₂ for insect farming. Cost of the gel isimportant, since it must be lower than the value of the increased yieldof the nutritional benefit of this biotechnology. To this effect, costscan be minimized by:

use of acidic food waste or acetic acid waste (0.25-7%) rather than highquality acetic acid for acidification;

use a minimum dose of glucomannan (e.g., 1.5-2.5%) alone or incombination with low dose maltodextrin (e.g., 0.5%);

use 10-100 mg of crude magnesium metal powder (Mg); and

water can be any water free of toxic metals, plasticizers, endocrinedisrupters and pesticides.

Example 25: Effect of Glucomannan on Generation and Sustaining MolecularHydrogen (H₂) in Aqueous Solutions—Bellow the Gelling Concentration

5. Introduction

A study was carried out, in an open ‘to the air’ container, to determineif low levels of glucomannan (gmn), below the gelation concentration,combined with magnesium metal powder (Mg*) can increase thesustainability of H₂ in Mg*-gmn aqueous solutions—relative to Mg*solutions—without glucomannan.

6. Experimental

Crystal Light® powder was used since previous experiments (Examples 10and 11 above) have demonstrated the effectiveness of the aqueous CrystalLight® media in supporting H₂ generation from Mg-gmn formulations.

Crystal Light® Natural Lemonade powder was mixed with all test powders,including the control without glucomannan. All formulations testedcontained 40 mg of 63-micron (230 Mesh) magnesium metal powder (Mg*) and1.9 g of Crystal Light® Natural Lemonade (CL). Crystal Light® Lemonadecontains citric acid, potassium citrate, sodium citrate, aspartame,magnesium oxide, maltodextrin, acesulfame potassium, soy lecithin,artificial color FD&C Yellow # 5, BHA and less than 2% natural flavor.

Six different test solutions were prepared containing 0.0, 0.15, 1.5,12, 100 and 1,000 mg of glucomannan (gmn). The Mg*-gmn plus CL powderswere combined and mixed. The formulations were then mixed with 100 mLdistilled water (DW) in a 250 mL glass beaker. Close to two-minutemixings took place. Immediately after mixing, measurements of molecularhydrogen (H₂) took place by immersing the Trustlex® H₂ Meter, withoutits guard cup, in the test solution until a steady reading was reached.Removing the guard cup allows un-impeded contact of the Trustlex®electrode with the gel.

Viscosity measurements on the control and test solutions took place witha #6 Zahn Viscosity Cup for testing the viscosity of Newtonian liquids.It can be used to measure the time, in seconds, for the test solutionsto flow out of the cup that is filled to its capacity.

7. Results

The results are shown in Table 14 and FIG. 1. In Column 2 of Table 14are displayed the time points at which H₂ measurements weretaken—starting right after two minutes of stirring a mixture.

TABLE 14 Time Course of Loss of Dissolved Molecular Hydrogen fromSolutions Containing Various Non-Gelling Levels of Glucomannan 3 5 7 911 13 gmn gmn gmn gmn gmn gmn 2 0 4 0.15 mg 6 1.5 mg 8 12 mg 10 0.1 g 121 g 14 1 Time H₂ % H₂ % H₂ % H₂ % H₂ % H₂ % Row Min. ppb Rem ppb Rem.ppb Rem. ppb Rem. ppb Rem ppb Rem. 1 0 807 100 785 100 800 100 808 100784 100 803 100 2 5 806 99.9 798 101.7 808 101.0 804 99.5 789 101 820102 3 10 812 100.6 804 102.4 809 101.0 804 99.5 790 101 824 103 4 15 814100.9 805 102.6 812 102.0 806 99.8 790 101 826 103 5 20 808 100.1 809103.1 814 102.0 806 99.8 793 101 828 103 6 30 802 99.4 808 1029 812102.0 806 99.8 789 101 825 103 7 40 798 98.9 806 102.7 810 101.0 80799.9 792 101 823 103 8 50 794 98.4 804 102.4 xxx xxx 806 99.7 791 101819 102.0 9 60 786 97.4 802 102.1 808 1.01 805 99.6 791 101 816 102 10120 646 80.0 758 96.6 784 98.0 790 98.3 783 99.9 802 99.8 11 180 43153.4 549 69.9 680 85.0 753 93.2 761 97.1 790 98.4 12 240 299 37.1 37948.3 440 55.0 592 73.3 686 87.5 789 98.3 13 300 201 24.9 234 29.8 32140.1 450 55.7 526 67.1 789 98.3 14 360 146 18.1 161 20.5 202 25.3 30938.2 394 50.3 802 99.9 Visc. (sec.) 1.2 xxx xxx 1.1 1.7 23.0Abbreviations % Rem. % dissolved H₂ remaining in solution - as measuredwith the Trustlex H₂ Meter. Visc. Viscosity Min. Minutes ppb parts perbillion H₂ molecular hydrogen gmn glucomannan g gram mg milligram sec.seconds

8. Control Formulation

Columns 3 and 4 of Table 14 show respectively, the parts per billion(ppb) and percent of dissolved H₂ remaining in solution due togeneration in the control formulation (i.e., 40 mg Mg*+1.9 g CL—withoutglucomannan). It is observed that there is an almost steady state levelof H₂ in solution up to one-hour after starting measurements. Thisphenomenon is clearly depicted in FIG. 1. This result, at first glance,is surprising, since experience in generating H₂ by electrolysis ofwater has shown a much more rapid rate of loss of H₂ from aqueoussolution. This persistence of H₂ in Mg*-generated H₂ solutions isattributed to continued generation of H₂, for a period of time after Mg*is mixed with water.

After one hour, there is a faster rate of loss of dissolved H₂ from thecontrol solution so that at 6-hours post preparation, only 18% of theoriginal amount of dissolved H₂ remains. Thus, it appears that there aretwo phases as is observed by analyzing FIG. 1: A ‘Steady State Phase’where dissolved H₂ is generated at approximately the same rate that itis lost to the environment, and a ‘Depletion Phase’, when dissolved H₂is lost to the environment at a faster rate than can be replaced by areaction of the unreacted Mg* with water.

9. Test Formulations

Formulations all containing 40 mg Mg*+1.9 g CL and also containingrespectively, 0.15, 1.5, 12, 100 mg and 1.0 g glucomannan mixed with 100mL of distilled water—were tested. At these low concentrations of gmn,viscous gels are not formed. The results presented in Columns 5, 7, 9,11 and 13 show the ppb of dissolved molecular hydrogen (H₂) remaining insolution—as a function of time. It is observed that there is adose-response relationship where glucomannan extends the ‘Steady State’Phase, beyond the 60-minute cut-off time found for the controlsolution—without glucomannan in the formulation. This phenomenon is seenby observing the results presented in FIG. 1. Even at the lowestconcentration of glucomannan tested (1.5 ppm), the ‘Steady State’ Phaseis shifted from lasting 1-hour to close to 2-hours. Formulationscontaining higher concentrations of gmn progressively increase thelength of the ‘Steady State’ Phase as can be seen by analyzing theresults in Columns 3-14 of Table 14 and FIG. 1. The results presented inColumns 13 and 14 of Table 14 and FIG. 1—show that the 40 mg Mg*+1.9 gCL formulation containing 1.0 g of gmn/100 mL DW extends the ‘SteadyState’ Phase to 360 minutes (6-hours) - and perhaps well beyond the6-hour time course of this Study. In fact, previously described studies(See Examples 4 and 5, above) attest to the long-term stability of H₂ inMg-gmn gels. However, as tested here, 40 mg of Mg*+1.9 g CL formulationscontaining, respectively, 0.15, 1.5, 12 and 100 mg of gmn/100 mL DWextend the ‘Steady State’ Phase without appreciably increasing theviscosity or forming a gel. The 40 mg Mg*+1.9 g CL formulationcontaining 1.0 g of gmn/100 mL DW modestly increases the viscosity,forming a viscous solution but does not form a viscous gel.

10. Discussion

Reviewing the results of the 1 to 6-hour time frame as depicted in Table14 and FIG. 1, it is observed that the ‘Steady State’ Phaseprogressively increases while the ‘Depletion Phase’ progressivelydecreases as the concentration of glucomannan is increased in the 40 mgMg*+1.9 g CL formulations. For the formulations containing 0.15 mg to upto 1.0 g of gmn, this remarkable stabilization of H₂ in the solutionscannot be due to a gelation effect. In an attempt to understand themechanism by which ‘below gelling concentrations’ of glucomannan sustainH₂ in 40 mg Mg*+1.9 g CL aqueous solutions, the following possibilitiesare considered:

gmn slows down the reaction of Mg* with water which generates H₂;

gmn has an affinity for H₂ which slows down its loss to the environmentfrom solution;

gmn stabilizes H₂ bubbles, in solution, thereby slowing down the rate ofloss from solution; or

gmn sustains the generation of H₂ in solution by removing thepassivation coat of magnesium oxide that is naturally found on magnesiummetal powder particles that have been exposed to oxygen.

Analysis of the data can eliminate possibility ‘1’ above. By observingthe results for the control solution in Columns 3-4, relative to theresults for the test solutions in Columns 5-14, it is seen that theinitial rate of reaction for producing H₂ is approximately equal to thatof the test solutions (See Row 1). Therefore, glucomannan does not slowdown the depletion of Mg and resultant H₂ production.

The idea that H₂ has an affinity for gmn is more than worthy ofconsideration. Copious visible bubbles are initially present in solutiondue to the generation of H₂ by magnesium metal powder. Stabilization ofthese bubbles in solution should create a reservoir of H₂ for dynamicexchange with dissolved H₂. This phenomenon should lead to increasedstabilization of H₂ in solution—compared to solutions containingdissolved H₂-without microbubbles. Accepting that H₂ has an affinity forgmn, it is reasonable to assume that non-gelling gmn molecules andcomplexes would be attracted to the H₂ bubble-water interface formingmore stable bubbles.

As discussed in Example 7, glucomannan can possibly catalyze the removalof the passivation coat of magnesium oxide from magnesium metal powderparticles, thereby increasing the efficiency of molecular hydrogenproduction. This mechanism can also play a role in sustaining molecularhydrogen in solutions containing glucomannan.

In summary, there are three mechanisms by which glucomannan can increasethe sustainability of molecular hydrogen in aqueous magnesium metalpowder solutions.

Example 26: Electrolysis Study: Sequestration of Molecular Hydrogen (H₂)by Glucomannan

11. Introduction

To test if there is an attractive interaction between H₂ andglucomannan, in aqueous solution—in the absence of magnesium metalpowder, an independent method of generating H₂ in glucomannan solutionwas sought. Electrolysis of water is a well-known means of generating H₂in solution. The reaction, at the electrodes, breaks down water into H₂and O₂. As discussed in the Background Section, above, water free ofelectrolytes, is needed to prevent chemical reactions that shorten the‘life’ of the electrodes. Use of water free of electrolytes, such asdistilled water, will generate H₂, but at a much slower rate than in thepresence of electrolytes.

It was decided to use electrolysis for generating H₂ in the presence andabsence of gmn. For this purpose, the loss of H₂ from solutions afterelectrolysis of neat distilled water as compared to the electrolysis ofdistilled water containing 120 ppm glucomannan—was performed.

12. Experimental

Five hundred ml of distilled water containing 62 mg of gmn was preparedin a 500 mL glass beaker by mixing and then heating to 65C to insure gmnsolubility. The mixture was then allowed to cool to room temperature (23C). Electrolysis of water took place in a 460 mL GX-H11 electrolysisbottle from Yongkang Gomax Ind. & Trade Co., Yogkang City, China. Thebottle has a working current of 1 Amp. with a DC12V/5V power supply.Electrolysis studies of both distilled water and 120 ppm gmn, indistilled water, were repeated.

13. Results

The time course of the electrolysis results is shown in Table 15. Column1 shows the time points of measurements after the start of the study.The results in Column 2 show the ppb of H₂ generated at each time pointafter completion of 6 minutes of electrolysis of distilled water (DW).Only 27 ppb of H₂ is present at the outset. As shown in Column 3 anddepicted in FIG. 2, at one-hour after completion of electrolysis, nodetectable H₂ remained in the electrolyzed solution. This is in accordwith previous observations that electrolysis of DW has a low yield of H₂which depends on the time course of the applied voltage—which isconstant for the studies described here.

TABLE 15 Effect of Glucomannan (gmn) on Molecular Hydrogen (H₂)Generation by Electrolysis in Distilled Water (DW) DW gmn Time (N = 3) %(N = 2) % min. ppb H₂ Change ppb H₂ Change 0 27 0 197 0 5 20 −26 235 1910 18 −33 241 22 20 17 −37 243 23 40 4 −85 223 13 60 0 −100 207 8 120xxx xxx 155 −21 180 xxx xxx 103 −48 240 xxx xxx 45 −77 Abbreviationsgmn—120 ppm glucomannan (0.012%) ppb—parts per billion H₂ min.—minutesafter starting H₂ measurements with the Trustlex Meter. H₂—Molecularhydrogen DW—Distilled water N—Number of repeats

The results presented in Column 4 and FIG. 2 show the ppb of H₂generated at each time point after completion of 6 minutes ofelectrolysis of distilled water containing 120 ppm glucomannan.Immediately after completion of electrolysis, 197 ppb of H₂ is detectedin the electrolyzed solution. H₂ then rises to 243 ppb at 20 minutesafter completion of electrolysis. This increase—relative toelectrolysis, without gmn, is attributed to an interaction of H₂ withgmn that helps retain H₂ in solution. Glucomannan, a polymer of glucoseand mannose, is not charged and should not directly affect electrolysis.At one-hour after completion of electrolysis, 207 ppb (85%) H₂ remainsin the electrolyzed solution. H₂ persists at 45 ppb at 4-hours aftercompletion of electrolysis.

14. Discussion

FIG. 2 contains a plot of the results that clearly shows the effect thata low dose (120 ppm) of glucomannan has on retaining H₂ insolution—without the presence of magnesium metal powder. Thus,glucomannan:

enhances the retention of H₂ in water that has been electrolyzed;

affects a rise in H₂ for at least 20 minutes after generation of H₂ insolution;

stabilizes H₂ in the solution—relative to generation of H₂ in DW.

Any method of making H₂ available to gmn should stabilize H₂ in aqueoussolution.

These results point to a strong interaction of H₂ with gmn, without thepresence of magnesium metal powder. Generation and subsequent infusionof molecular hydrogen from a canister or electrolysis of water deviceinto an aqueous solution containing glucomannan is another means bywhich glucomannan can interact with H₂ and stabilize H₂ in solution.

Electrolysis devices have been discussed previously. From the resultspresented here, these devices could be used to deliver H₂ to solutionscontaining gmn. Longer times of electrolysis and higher concentrationsof gmn would increase the stability of H₂ in aqueous solutions.

Using a commercial source of H₂ to deliver H₂ to glucomannan solutionsis another method to consider. Canisters containing pressurized H₂ arecommercially available from Restek (34453-PI-Hydrogen; $724.94). H₂generators such as Zen Earth (HX300 Hydrogen Machine—around $2,500) andParker Hydrogen Generator ($10,000-17,000) are also commerciallyavailable. These devices can readily be located on the interne. Thesecanisters and devices can be used to diffuse or pressurize H₂ intoglucomannan solutions. They provide another reliable source of H₂. Thedisadvantages are cost and a safety issue—if the level of H₂ in thesurrounding atmosphere reaches 4% v/v or higher.

Another application of the Invention is the sequestration and storage ofH₂ from environmental sources. This application would be particularlyimportant in third world countries in need of an inexpensive source ofenergy. H₂ is a well-known source of energy as well as administered forimproving health. H₂ is produced, in quantity, mostly by microbialanaerobic metabolism: in wastewater; wastewater plants; parts of theocean—by sea life including cyanobacteria; swamps; the gastrointestinaltracts of animals and humans. Passing hydrogen or solutions containingH₂ through gmn solutions or filters containing gmn—will result insequestration of H₂ that can be recovered for energy use.

Example 27: Electrolysis of Water in the Presence of 0.05% K Bicarbonateand Glucomannan

It is well known that addition of sodium or potassium bicarbonate to‘pure’ water such as distilled water, will increase the output of H₂ dueto electrolysis. However, keeping the concentration of bicarbonate lowis desirable due to its ‘off taste’, as well as keeping sodium orpotassium from reaching a level that is detrimental to health ofindividuals as well as the electrodes.

Since it has been shown that 120 ppm glucomannan (gmn) enhances H₂generation and sustainability in electrolyzed distilled water (See Table15), an electrolysis experiment was designed to determine if there issuch an effect on generation of H₂ when 120 ppm gmn is added to 0.05%potassium bicarbonate.

The results are shown in Table 16. The first column lists the timecourse of the Study. Column 2 shows the change in H₂ generated byelectrolysis of the K bicarbonate solution as time progresses. In thefirst 10 minutes, H₂ rises by 4% and then progressively falls to losing52% of H₂ at 3 hours and 95% of H₂ at 7-hours.

TABLE 16 Effect of Glucomannan (gmn) on Molecular Hydrogen (H₂)Generation by Electrolysis of K bicarbonate in Distilled Water (DW)0.05% K 0.05% K bicarbonate, bicarbonate 120 ppm gmn Time in DW % in DW*% min. ppb Chg ppb Chg 0 575 −4 541 −7 5 591 −1 580 xxx 10 596 xxx 565−3 20 575 −4 566 −3 40 554 −7 546 −6 60 518 −13 528 −9 120 395 −34 461−21 180 289 −52 406 −30 240 214 −64 347 −40 420 32 −95 133 −77 pH 8.787.90 Abbreviations: gmn—120 ppm glucomannan (0.012%) Ch—Change in H₂ insolution ppb—parts per billion H₂ min. minutes after starting H₂measurements with the Trustlex Meter. H₂—Molecular hydrogen DW—Distilledwater

Column 4 shows the time course of H₂ changes after 6 minutes (3minutes×2) of electrolysis of 120 ppm gmn+0.05% K bicarbonate in DW. Theresults were normalized for differences in pH—to those of Column 2 -using the Nernst equation. Comparing the results in Column 4 with thosein Column 2, it is observed that a similar pattern of H₂ increasing from0 to 5-minutes, followed by a progressive decrease of H₂ in solution.However, there is a marked stabilization of H₂, in the electrolyzedsolution containing gmn with 0.05% K bicarbonate—relative to theelectrolysis of 0.05% K bicarbonate solution. After 60 minutes, thiseffect becomes more obvious. For example, at 2-hours after the start ofthe study, there is a 16.1% increase in H₂ in the electrolytic solutioncontaining 120 ppm gmn while at 7 hours after the start of the study,there is a 416% increase. These results point to microbubbles beingpresent in the electrolysis solution containing 120 ppm glucomannan.

Example 28: Optical Microscopy Detection of H₂ Microbubbles

Due to the unexpected enhanced sustainability of H₂ in both aqueousmagnesium metal powder and electrolysis systems containing glucomannan(gmn), a study was carried out to determine if significant amounts ofmicrobubbles are present in a solution showing enhanced H₂ stability.The formulation investigated contained 44 mg Mg*, 120 ppm gmn, 1.9 gCrystal Light® Natural Lemonade powder mixed into 100 mL distilledwater. After mixing for 60 seconds in an 8 oz. cup, the formulation wasallowed to stand at 23 C for 4.5-hours before filtration and testing.The formulation was filtered through a 400-mesh filter (ATPWONZ FoodStrainer) which provides for a larger than 37-micron particle sizeretention in the filter. Therefore, all microbubbles passing through the400 Mesh filter were 37 microns or smaller. Thereafter, 20 uL of thefiltered solution was injected onto the sintered glass space adjacent tothe glass coverslip covering the grid on a hemocytometer. The grid wasobserved under the 40/0.065 magnification on the OMAX® BinocularCompound Microscope Model: M83EZ.

At the 4.5-hour observation, numerous microbubbles were observed, asshown in FIG. 3. Here a wide range of sizes (diameters) are observed.Since the largest size is 37 microns, then the smaller size rangesobserved must range between 2-10 microns.

At 8.5-hours, the filtered formulation was refreshed by cleaning anddrying the hemocytometer and injecting 20 uL of the solution onto thesintered glass space adjacent to the glass coverslip—covering the gridon the hemocytometer. A wide range of microbubbles of assorted sizes isobserved. Thus, the microbubbles observed, have a sustainability of atleast 8.5 hours in the 44 mg Mg*, 120 ppm glucomannan, Crystal Light ®formula. These results are in accord with the results shown in Columns 9and 10 of Table 15 - where it is seen that 309 ppm H₂ (38.2%) is present6-hours after preparation of a 40 mg Mg*, 120 ppm glucomannan, CrystalLight® solution.

From the results presented in FIGS. 3-4 and Tables 15-17, there isconvincing evidence that the persistence of H₂ in non-viscous solutionscontaining glucomannan is due to the stabilization of microbubbles byaqueous glucomannan.

Variable quantities of H₂ bubbles in non-viscous glucomannan (gmn)solutions can be generated and controlled by:

Electrolysis of aqueous 0.5 ppm-1,000 ppm gmn solutions: Extending theelectrolysis time and/or voltage, and the presence of bicarbonateelectrolytes will increase bubble formation, including microbubbles.Other electrolytes are not recommended due to their adverse effects onthe lifetime of the electrodes.

Reaction of magnesium metal powder (Mg) with water in acidic 0.5ppm-1,000 ppm gmn solutions. Increasing the concentration of Mg, e.g., 1mg-1000 mg per 100 mL , will increase the generation of H₂ bubblesstabilized by glucomannan.

Using a hydrogen canister for diffusing or pressurizing H₂ into aqueous0.5 ppm-1,000 ppm gmn solutions. This method requires a source of H₂,such as a canister, to be available for use.

Using a hydrogen generator (e.g., Parker Hannifin 20h hydrogen generatorcapable of 160 mL H₂/min.

Direct water splitting through vibrating piezoelectric zinc oxidemicrofibers in aqueous 0.5 ppm-1,000 ppm gmn solutions.

The size of the H₂ microbubbles in H₂-generating systems can be selectedby:

Molecular sieving, e.g., passing a solution through a 1250 Mesh filterwill allow 10 micron or smaller microbubbles to pass.

Centrifugation where larger bubbles are removed before the microbubbles.The time and speed of centrifugation is contingent on the bubble sizecut-off desired.

Size exclusion chromatography where the microbubbles readily passthrough the column while the larger bubbles are held back.

The ability to generate sufficient quantities of stable H₂ microbubblesin aqueous solution has important health benefits regarding enhancingultrasonic biotechnology:

ultrasonic imaging of organs and the circulatory system of humans andlower life forms;

ultrasonic drug delivery, including chemotherapy, to specific organs,including crossing the blood-brain barrier;

treatment of prostate cancer, histotripsy (mechanical tissuefractionation using high frequency ultrasound) and sonothrombolysis(removal of blood clots using sound waves);

ultrasonic delivery of macromolecules including DNA, RNA and proteins tospecific tissues, including enhancement of CRSPR biotechnology.

vascular permeability enhancement;

lithotripsy, the disintegration of kidney and bladder stones; or

the benefits listed above, plus the delivery of antioxidant andanti-inflammatory efficacy due to H₂.

Example 29: Sequestration of Molecular Hydrogen (H₂) from Water Flowingthrough a Filter Containing a Glucomannan Gel

15. Introduction

There is a need for an inexpensive source of clean energy in poor, thirdworld environments. These environments usually have an abundance ofwastewater. Anaerobic fermentation of wastewater generates copiousamounts of both H₂ and CO₂ as well as methane. A method has been devisedby which an aqueous glucomannan gel can be used to sequester H₂ fromflowing waste-water and simultaneously-separate it from carbon dioxide.It is noted the konjac plant that contains glucomannan is often farmedin some third-world countries. In such places, it would be costeffective to use glucomannan for sequestering H₂ from wastewater.

16. Results

The drawing in FIG. 5A depicts a preformed aqueous 3-10% glucomannan gel(520) placed in a filter casing (530) that allows 20 -50% expansion ofthe gel in the casing. The gel is preformed around 20-100 plastic ormetal rods, 2-4-cm in diameter, so that pores (510) extend from one endof the gel to the other after the gel forms and the rods are withdrawn.Filter casings can be ‘off the shelf’ products. Gels can be sizedaccording to the needs for sequestering of H₂.

FIG. 5B depicts the filter casing (550) comprising the aqueousglucomannan gel for sequestering H₂ from a stream of water flowing intothe canister through an intake port (560). Water is exposed to theglucomannan gel and within the canister and flows out through the outputport (540). The diagram in FIG. 6 is descriptive: 1)waste water ispressurized into the system by gravity or a pump; 2) large particlesand/or sludge is removed from the water stream by Prefilter #1 (670)which can comprise inexpensive and reversibly cleaned sand; 3) smallparticles, metals and organic compounds are removed from the stream byPrefilter #2 (680) which can comprise zeolites as well as other suchsequestering materials; and 4) water flows into Filter #3 (650),comprising the aqueous glucomannan gel, water flows into the gel throughthe pores and around the gel until the gel expands due to itssequestration of H₂, hereafter, the water flows through the gel, H₂ isremoved, sequestered and stored in the expanded aqueous glucomannan gel;5) the H₂-glucomannan gel can be degassed by heating, or otherwise toproduce H₂ gas for energy or health use; and 6) the aqueous glucomannangel can be recycled to the filter casing, to collect additional cyclesof H₂. Filters are connected in series, by non-limiting example, withconnectors (690).

17. Discussion.

As shown in Example 6 (above), aqueous glucomannan gels sequester H₂ butnot carbon dioxide. Therefore, the H₂ sequestered by the aqueousglucomannan gel will not be ‘poisoned’ by carbon dioxide. That is,carbon dioxide will not be present to extinguish the flammability of thesequestered H₂. On the other hand, if the aqueous glucomannan gelsequesters some methane, it will not present a problem since methane,like H₂, can be burned for energy.

Example 30: Effect of Varying Magnesium Metal Powder on thePhysical-Chemical Properties of a Weight Loss Product

18. Introduction

Volume and viscosity are two properties of a gel formulation that canimpart a feeling of fullness when residing in the stomach. Increases inboth volume and viscosity will enhance the experience of satiety.

A study was carried out to determine the effect of increasing theconcentration of magnesium metal powder (Mg*) on the viscosity, volume,molecular hydrogen content and related physical-chemical properties of alemon-flavored weight loss formulation.

19. Experimental

Table 17 contains a list of ingredients in the formulations. As shown,the Mg* concentration was varied from 0, 0.12, 0.24 to 0.48 g in therespective formulations. Gels were prepared by adding 4.0 grams of eachformulation to 400 mL of distilled water and mixing with a utensil for120 seconds. The resultant gels were allowed to stand at 70 deg. F for1-hour.

TABLE 17 Effect of Varying Magnesium Metal Powder on the Physical -Chemical Properties of a Weight Loss Product Formula Ingredients/400 mLDistilled Water Grams Ingredient Purpose 8.00 ErythritolSweetener/Filler 7.00 L-citric acid - anhydrous Lemon Flavor 5.20 Konjacglucomannan Viscosity Builder 2.00 Xanthan gum Thickener 1.20 sodiumascorbate antioxidant/preserve 0.92 Magnesium sulfate Anti-caking 0.72sucralose sweetener Variable 230 Mesh Magnesium metal Generate H₂ powder(MMP) 0.16 Vitamin E Powder antioxidant/preserve 0.02 Riboflavin ColorDens. Vol MMP (g/mL) (mL) Viscosity H₂ pH 0 1.050 405 17,400 0 2.62 0.120.859 495 34,200 629 2.93 0.24 0.810 525 90,500 715 3.00 0.48 0.709 60078,500 585 3.14 Abbreviations MMP Magnesium metal powder passing througha 230 Mesh sieve. Dens. Density g grams mL milliliters Vol. Volume H₂molecular hydrogen measured with the Trustlex Meter.

Volumes were determined by the height of gel attained in the 600 mLbeaker. Viscosities were measured with an NDJ-1 rotary type viscometer.For the control gel, not containing Mg*, which had the lowest viscosity,Rotor #3 at a rotation rate of 6 rpm was used. For the threeformulations containing Mg*, Rotor #4 and at a rotation rate of 12 rpmwas used. The dissolved molecular hydrogen persisting in the gels, afterstanding for 1-hour, was measured with the Trustlex® H₂ Meter. pH wasmeasured with a calibrated ExStick II pH meter. Gel density wascalculated by dividing the total weight of each gel by its volume—aslisted in Column 14.

20. Results and Discussion

Increasing the concentration of Mg* in the weight loss formulation,depicted in Column 1 of Table 17, results in a concomitant increase ingel volume (see Column 3 of Table 17). This increase in gel volume isdue to the generation of molecular hydrogen (H₂). This increase involume results in a decrease in gel density as shown in Column 2 ofTable 17.

Viscosity measurements indicate a more complex picture, where thepresence of Mg* markedly increases the viscosity—relative to theControl—without Mg* (Column 4 of Table 17). However, a maximum viscosityis reached at an intermediate concentration, i.e., at a concentration of0.24 g Mg*. Also, this is the gel that retains the highest concentrationof dissolved H₂. In contrast, the pH of the gels increases as theconcentration of Mg* in the gels increases—due to the formation ofmagnesium hydroxide due to the reaction of Mg* with water.

The results are best explained by: As H₂ is generated in the gelscontaining Mg*, the gels retain H₂ bubbles by a strong interaction withglucomannan in the gels. As the density is decreased to 0.810 g/mL,there is a parallel increase in viscosity due to the interaction of H₂bubbles with the gel matrix. This effect is conducive to retainingdissolved H₂, as well. As the volume increases beyond 525 mL, the gelbecomes more porous, allowing a greater escape of dissolved H₂ as wellas a relative decrease in gel viscosity.

In summary, the optimal gel for affecting satiety—is the gel containing0.24 g of Mg*/400 mL distilled water. While preferred embodiments of thepresent invention have been shown and described herein, it will beobvious to those skilled in the art that such embodiments are providedby way of example only. Numerous variations, changes, and substitutionswill now occur to those skilled in the art without departing from theinvention. It should be understood that various alternatives to theembodiments of the invention described herein may be employed inpracticing the invention. It is intended that the following claimsdefine the scope of the invention and that methods and structures withinthe scope of these claims and their equivalents be covered thereby.

1-25. (canceled)
 26. A powder composition comprising glucomannan, and abase metal powder.
 27. The powder composition of claim 26, wherein, uponmixing the powder composition with a composition comprising an aqueoussolvent having an acidic pH, the resulting composition forms a hydrogelor a flowable liquid or a cream or a lotion.
 28. The powder compositionof claim 26, wherein the glucomannan comprises from about 0.01% to about99.00% w/w of the powder composition.
 29. The powder composition ofclaim 27, wherein the resulting composition comprises gaseous H₂ anddissolved H₂.
 30. The powder composition of claim 26, wherein the basemetal powder comprises: a different base metal powder than magnesiummetal powder; a combination of magnesium metal powder with another basemetal powder; one or more additional base metals selected from the groupconsisting of lithium, potassium, strontium, calcium, sodium, aluminum,zinc, chromium, manganese, iron; or any combination thereof.
 31. Thepowder composition of claim 26, further comprising an organic acid. 32.The powder composition of claim 26, further comprising an organic acid,wherein the resulting composition has an acidic pH.
 33. The compositionof claim 32 wherein the organic acid is selected from the listconsisting of citric acid, malic acid, lactic acid, acetic acid,tartaric acid, succinic acid, phosphoric acid, formic acid, oxalic acid,uric acid, ascorbic acid and any combination thereof.
 34. The powdercomposition of claim 26, wherein the composition further comprising oneor more excipients selected from the list consisting of sweeteners,antioxidants, anticaking agents, flavoring agents, coloring agents, orany combination thereof.
 35. The powder composition of claim 26, whereinthe powder composition is enclosed in a capsule to form an encapsulatedcomposition.
 36. The encapsulated composition of claim 35, wherein theencapsulated composition is enclosed in the capsule that is 000 in size.37. The encapsulated composition of claim 35, wherein the encapsulatedcomposition is enclosed in the capsule comprising cellulose.
 38. Thecomposition of claims 26, wherein the composition is contained in asingle dose for addition to a composition comprising an aqueouscomposition to generate a molecular hydrogen containing cream or lotion.39. The composition of claim 38, wherein the aqueous compositioncomprises at least 100 ppb molecular hydrogen.
 40. The composition ofclaim 26, wherein the compositions comprise vitamins or minerals, aloneor in combination.
 41. The composition of claim 40, wherein the vitaminsor minerals alone or in combination are in an amount of about 5% toabout 15% of RDI (required Daily Intake) for a healthy adult human. 42.The composition of claim 41, wherein the vitamins or minerals, alone orin combination are in an amount of about 5% to about 100% of the RDI.43. The composition of claim 27, wherein the composition is adapted forapplication to the skin of a subject.
 44. The composition of claim 27,wherein the composition provides a moisturizing effect to the skin of asubject.
 45. The powder composition of claim 26, wherein the base metalpowder comprises magnesium metal powder.